Fast-Curing of Liquid Crystal Thermosets Enabled by End-Groups Regulation and In Situ Monitoring by Triboelectric Spectroscopy.

The development of high-performance polymer is crucial for the fabrication of triboelectric nanogenerators (TENGs) used in extreme conditions. Liquid crystal polyarylate thermosets (LCTs) demonstrate great potential as triboelectric material by virtue of exceptional comprehensive properties. However, there are only a few specific end-groups like phenylethynyl matching the LCT polycondensation temperature (above 300 °C). Moreover, the excellent properties of LCTs rely on the crosslinked network formed with long curing time at high temperature, restricting their further application in triboelectric material. Herein, a fast-curing LCT is designed by terminating with 4-maleimidophenol possessing appropriate reactivity. The resultant LCT (MA-LC-MA) exhibits much lower polycondensation temperature (250-270 °C) and curing temperature of 300 °C within only 1 min compared to typical LCTs (cured at 370 °C for 1 h). Furthermore, the cured MA-LC-MA retains a high glass transition temperature of 135 °C, storage modulus of 6 MPa even at 350 °C, and great electrical output performance. Additionally, triboelectric measurement related to the dielectric properties that vary with crosslinked network is innovatively utilized as an analysis technique of curing progress. This work provides a new strategy to design high-performance TENGs and promotes the development of next generation thermosets in extreme conditions.

A fluorine-based strong and healable elastomer with unprecedented puncture resistance for high performance flexible electronics.

There is usually a trade-off between high mechanical strength and dynamic self-healing because the mechanisms of these properties are mutually exclusive. Herein, we design and fabricate a fluorinated phenolic polyurethane (FPPU) elastomer based on octafluoro-4,4'-biphenol to overcome this challenge. This fluorine-based motif not only tunes interchain interactions through π-π stacking between aromatic rings and free-volume among polymer chains but also improves the reversibility of phenol-carbamate bonds via electron-withdrawing effect of fluorine atoms. The developed FPPU elastomer shows the highest recorded puncture energy (648.0 mJ), high tensile strength (27.0 MPa), as well as excellent self-healing efficiency (92.3%), along with low surface energy (50.9 MJ m-2), notch-insensitivity, and reprocessability compared with non-fluorinated counterpart biphenolic polyurethane (BPPU) elastomer. Taking advantage of the above-mentioned merits of FPPU elastomer, we prepare an anti-fouling triboelectric nanogenerator (TENG) with a self-healable, and reprocessable elastic substrate. Benefiting from stronger electron affinity of fluorine atoms than hydrogen atoms, this electronic device exhibits ultrahigh peak open-circuit voltage of 302.3 V compared to the TENG fabricated from BPPU elastomer. Furthermore, a healable and stretchable conductive composite is prepared. This research provides a distinct and general pathway toward constructing high-performance elastomers and will enable a series of new applications.

An Encapsulation-Free and Hierarchical Porous Triboelectric Scaffold with Dynamic Hydrophilicity for Efficient Cartilage Regeneration.

Tissue engineering and electrotherapy are two promising methods to promote tissue repair. However, their integration remains an underexplored area, because their requirements on devices are usually distinct. Triboelectric nanogenerators (TENGs) have shown great potential to develop self-powered devices. However, due to their susceptibility to moisture, TENGs have to be encapsulated in vivo. Therefore, existing TENGs cannot be employed as tissue engineering scaffolds, which require direct interaction with surrounding cells. Here, the concept of triboelectric scaffolds (TESs) is proposed. Poly(glycerol sebacate), a biodegradable and relatively hydrophobic elastomer, is selected as the matrix of TESs. Each hydrophobic micropore in multi-hierarchical porous TESs efficiently serves as a moisture-resistant working unit of TENGs. Integration of tons of micropores ensures the electrotherapy ability of TESs in vivo without encapsulation. Originally hydrophobic TESs are degraded by surface erosion and transformed into hydrophilic surfaces, facilitating their role as tissue engineering scaffolds. Notably, TESs seeded with chondrocytes obtain dense and large matured cartilages after subcutaneous implantation in nude mice. Importantly, rabbits with osteochondral defects receiving TES implantation show favorable hyaline cartilage regeneration and complete cartilage healing. This work provides a promising electronic biomedical device and will inspire a series of new in vivo applications.

Bone-inspired stress-gaining elastomer enabled by dynamic molecular locking.

The limited capacity of typical materials to resist stress loading, which affects their mechanical performance, is one of the most formidable challenges in materials science. Here, we propose a bone-inspired stress-gaining concept of converting typically destructive stress into a favorable factor to substantially enhance the mechanical properties of elastomers. The concept was realized by a molecular design of dynamic poly(oxime-urethanes) network with mesophase domains. During external loading, the mesophase domains in the condensed state were aligned into more ordered domains, and the dynamic oxime-urethane bonds served as the dynamic molecular locks disassociating and reorganizing to facilitate and fix the mesophase domains. Consequently, the tensile modulus and strength were enhanced by 1744 and 49.3 times after four cycles of mechanical training, respectively. This study creates a molecular concept with stress-gaining properties induced by repeated mechanical stress loading and will inspire a series of innovative materials for diverse applications.

Hybrid Hydrogen Bonding Strategy to Construct Instantaneous Self-Healing Highly Elastic Ionohydrogel for Multi-Functional Electronics.

Gels show great promise for applications in wearable electronics, biomedical devices, and energy storage systems due to their exceptional stretchability and adjustable electrical conductivity. However, the challenge lies in integrating multiple functions like elasticity, instantaneous self-healing, and a wide operating temperature range into a single gel. To address this issue, a hybrid hydrogen bonding strategy to construct gel with these desirable properties is proposed. The intricate network of hybrid strong weak hydrogen bonds within the polymer matrix enables these ionohydrogel to exhibit remarkable instantaneous self-healing, stretching up to five times their original length within seconds. Leveraging these properties, the incorporation of ionic liquids, water, and zinc salts into hybrid hydrogen bond crosslinked network enables conductivity and redox reaction, making it a versatile ionic skin for real-time monitoring of human movements and respiratory. Moreover, the ionohydrogel can be used as electrolyte in the assembly of a zinc-ion battery, ensuring a reliable power supply for wearable electronics, even in extreme conditions (-20 °C and extreme deformations). This ionohydrogel electrolyte simplifies the diverse structural requirements of gels to meet the needs of various electronic applications, offering a new approach for multi-functional electronics.

4D Printed Non-Euclidean-Plate Jellyfish Inspired Soft Robot in Diverse Organic Solvents.

Soft robots have the potential to assist and complement human exploration of extreme and harsh environments (i.e., organic solvents). However, soft robots with stable performance in diverse organic solvents are not developed yet. In the current research, a non-Euclidean-plate under-liquid soft robot inspired by jellyfish based on phototropic liquid crystal elastomers is fabricated via a 4D-programmable strategy. Specifically, the robot employs a 3D-printed non-Euclidean-plate, designed with Archimedean orientation, which undergoes autonomous deformation to release internal stress when immersed in organic solvents. With the assistance of near-infrared light illumination, the organic solvent inside the robot vaporizes and generates propulsion in the form of bubble streams. The developed NEP-Jelly-inspired soft robot can swim with a high degree of freedom in various organic solvents, for example, N, N-dimethylformamide, N, N-dimethylacetamide, tetrahydrofuran, dichloromethane, and trichloromethane, which is not reported before. Besides bionic jellyfish, various aquatic invertebrate-inspired soft robots can potentially be prepared via a similar 4D-programmable strategy.

High Performance and Reprocessable In Situ Generated Nanofiber Reinforced Composites Based on Liquid Crystal Polyarylate.

Polymers are playing important roles in the rapid development of triboelectric nanogenerators (TENGs); However, most polymers cannot meet the high requirements of thermomechanical performance; Thus, various polymeric composites are developed for triboelectric layer. These composites are hardly recycled since their reinforcements are unevenly distributed after reprocessing, which limits the sustainable development of TENGs. To solve the above challenges, in situ generated nanofiber reinforced composites (NFRCs) based on single-component liquid crystal polyarylate (LCP) are designed and prepared via a one-step polycondensation. Nonlinear naphthalene (NDA) widens the processing window of LCP without destabilizing the liquid crystal phase. The NDA-rich domains act as a matrix while the NDA-poor domains with higher rigidity form oriented nanofibers to achieve self-reinforcement. The resultant NFRCs possess high glass transition temperature (Tg > 220 °C) and storage modulus (E' = 0.1 GPa at 350 °C), which are far beyond existing triboelectric polymers, typically Tg < 110 °C and E' < 0.1 MPa (flowable) at 350 °C. Furthermore, NFRC-based TENG exhibits superior electrical output performance and retention rate (>90%) after reprocessing; Overall, this work offers a new design principle to prepare self-reinforced composites, which paves a way to explore high performance materials.

Spider-Silk-Inspired Tough, Self-Healing, and Melt-Spinnable Ionogels.

As stretchable conductive materials, ionogels have gained increasing attention. However, it still remains crucial to integrate multiple functions including mechanically robust, room temperature self-healing capacity, facile processing, and recyclability into an ionogel-based device with high potential for applications such as soft robots, electronic skins, and wearable electronics. Herein, inspired by the structure of spider silk, a multilevel hydrogen bonding strategy to effectively produce multi-functional ionogels is proposed with a combination of the desirable properties. The ionogels are synthesized based on N-isopropylacrylamide (NIPAM), N, N-dimethylacrylamide (DMA), and ionic liquids (ILs) 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMI][TFSI]). The synergistic hydrogen bonding interactions between PNIPAM chains, PDMA chains, and ILs endow the ionogels with improved mechanical strength along with fast self-healing ability at ambient conditions. Furthermore, the synthesized ionogels show great capability for the continuous fabrication of the ionogel-based fibers using the melt-spinning process. The ionogel fibers exhibit spider-silk-like features with hysteresis behavior, indicating their excellent energy dissipation performance. Moreover, an interwoven network of ionogel fibers with strain and thermal sensing performance can accurately sense the location of objects. In addition, the ionogels show great recyclability and processability into different shapes using 3D printing. This work provides a new strategy to design superior ionogels for diverse applications.

Continuous Melt Spinning of Adaptable Covalently Cross-Linked Self-Healing Ionogel Fibers for Multi-Functional Ionotronics.

Stretchable conductive fibers play key roles in electronic textiles, which have substantial improvements in terms of flexibility, breathability, and comfort. Compared to most existing electron-conductive fibers, ion-conductive fibers are usually soft, stretchable, and transparent, leading to increasing attention. However, the integration of desirable functions including high transparency, stretchability, conductivity, solvent resistance, self-healing ability, processability, and recyclability remains a challenge to be addressed. Herein, a new molecular strategy based on dynamic covalent cross-linking networks is developed to enable continuous melt spinning of the ionogel fiber with the aforementioned properties. As a proof of concept, adaptable covalently cross-linked ionogel fibers based on dimethylglyoximeurethane (DOU) groups (DOU-IG fiber) are prepared. The resultant DOU-IG fiber exhibited high transparency (>93%), tensile strength (0.76 MPa), stretchability (784%), and solvent resistance. Owing to the dynamic of DOU groups, the DOU-IG fiber shows high healing performance using near-infrared light. Taking advantage of DOU-IG fibers, multifunctional ionotronics with the integration of several desirable functionalities including sensor, triboelectric nanogenerator, and electroluminescent display are fabricated and used for motion monitoring, energy harvesting, and human-machine interaction. It is believed that these DOU-IG fibers are promising for fabricating the next generation of electronic textiles and other wearable electronics.

An Intrinsically Magnetic Epicardial Patch for Rapid Vascular Reconstruction and Drug Delivery.

Myocardial infarction (MI) is a major cause of mortality worldwide. The major limitation of regenerative therapy for MI is poor cardiac retention of therapeutics, which results from an inefficient vascular network and poor targeting ability. In this study, a two-layer intrinsically magnetic epicardial patch (MagPatch) prepared by 3D printing with biocompatible materials like poly (glycerol sebacate) (PGS) is designed, poly (ε-caprolactone) (PCL), and NdFeB. The two-layer structure ensured that the MagPatch multifariously utilized the magnetic force for rapid vascular reconstruction and targeted drug delivery. MagPatch accumulates superparamagnetic iron oxide (SPION)-labelled endothelial cells, instantly forming a ready-implanted organization, and rapidly reconstructs a vascular network anastomosed with the host. In addition, the prefabricated vascular network within the MagPatch allowed for the efficient accumulation of SPION-labelled therapeutics, amplifying the therapeutic effects of cardiac repair. This study defined an extendable therapeutic platform for vascularization-based targeted drug delivery that is expected to assist in the progress of regenerative therapies in clinical applications.

Hybrid Cross-Linking to Construct Functional Elastomers.

ConspectusElastomers have been extensively used in diverse industrial sectors such as footwear, seals, tires, and cable jacketing and have attracted more and more attention in emerging fields such as regenerative medicine, soft robotics, and stretchable electronics. Global consumption of natural and synthetic elastomers amounted to nearly 27 million metric tons in 2020. In addition, to further enhance the common properties of elastomers, it is highly desired to endow elastomers with functionalities such as reprocessability, biomimetic mechanical properties, self-healing ability, bioactivity, and electrical conductivity, which will significantly broaden their applications. The covalent or noncovalent cross-linked structure is the essential factor for the elasticity of elastomers. Traditional elastomers usually comprise a single type of cross-linked molecular network, for which it is difficult to modulate the properties and introduce functionalities. Inspired by the simultaneous existence of multiple cross-linked structures in proteins, researchers have employed a hybrid cross-linking strategy to construct elastomers. Various noncovalent interactions (e.g., hydrogen bonds, metal-ligand coordination, ionic interactions, and chain folding) and dynamic covalent bonds (e.g., disulfide bonds, oxime-urethane bonds, and urea bonds) have been integrated in elastomers. Accordingly, the properties and functionalities of elastomers can be tuned by regulating the types, ratios, and distributions of cross-links. The hybrid cross-linking strategy provides a versatile and effective way to construct diverse functional elastomers for broad applications in various important fields.In this Account, we present our recent progress on functional elastomers constructed by a hybrid cross-linking strategy, including their design, preparation, properties, and diverse applications. First, we provide a brief introduction of the basic concept of functional elastomers and outline general strategies and mechanics for functional elastomers constructed by hybrid cross-linking. Then, we classify hybrid cross-linked elastomers by their design strategies, including multiple cross-linking, topological design, chemical coupling, and multiple networks. The relationships between the functionalities and hybrid cross-linked structures are summarized. At the same time, we also introduce diverse applications of these hybrid cross-linked elastomers in biomedicine, flexible electronics, soft robotics, 3D printing, and so on. Finally, we discuss our perspective on open challenges and future development trends of this rapidly evolving field. This Account highlighting the diverse hybrid cross-linked elastomers not only provides insights into strategies for elastomer functionalization but also provides new ideas for material design and inspires a variety of new applications.

Near-Infrared Light Triggered the Shape Memory Behavior of Polydopamine-Nanoparticle-Filled Epoxy Acrylate.

Through the effective combination of photothermal conversion agent polydopamine (PDA) nanoparticles and epoxy acrylate polymer (EA), a new kind of near-infrared (NIR) light-triggered shape memory polymer (PDA/EA) is developed. Due to the outstanding photothermal effect of PDA, even with a very low concentration of PDA (0.1 wt.%), when exposed to an 808 nm NIR light with a power of 1 W/cm2, the temporary shapes can be fully light-responsive, recovered in 60 s. Based on dynamic thermomechanical analysis and thermal gravimetric analysis, it can be seen that the introduction of PDA is beneficial for improving dynamic mechanical properties and thermal resistance compared to EA. As an environmentally friendly and highly efficient photoactive SMP, PDA/EA has a great application prospect.

The Relationships between the Structure and Properties of PA56 and PA66 and Their Fibers.

Bio-based polymers can reduce dependence on nonrenewable petrochemical resources and will be beneficial for future sustainable developments due to their low carbon footprint. In this work, the feasibility of bio-based polyamide 56 (PA56) substituting petroleum-based PA66 is systematically investigated. The crystallization, melting, and decomposition temperature of PA56 were all lower than that of PA66. PA56 formed a γ crystal type with larger grain size and took a longer amount of time to complete the crystallization process since its crystallization rate was lower than that of PA66. Compared with PA66, PA56 exhibited a higher tensile strength of 71.3 ± 1.9 MPa and specific strength of 64.8 ± 2.0 MPa but lower notched impact strength. More importantly, the limited oxygen index and vertical combustion measurement results indicated that the flame retardancy of PA56 was better than PA66, and the LOI values and the UL94 result of PA56 were 27.6% ± 0.9% and V-2. It is worth noting that the PA56 fiber had superior biodegradability compared to the PA66 fiber. PA56 showed significant biodegradation from the eighth week, whereas PA66 remained clean until the sixteenth week (without obvious biodegradation taking place). Eventually, PA56 did not show significant differences compared to PA66 in terms of thermal and mechanical properties. However, PA56 had great advantages in flame retardancy and biodegradability, indicating that the bio-based PA56 could potentially replace petroleum-based PA66 in many fields.

3D Printed Chondrogenic Functionalized PGS Bioactive Scaffold for Cartilage Regeneration.

Tissue engineering is emerging as a promising approach for cartilage regeneration and repair. Endowing scaffolds with cartilaginous bioactivity to obtain bionic microenvironment and regulating the matching of scaffold degradation and regeneration play a crucial role in cartilage regeneration. Poly(glycerol sebacate) (PGS) is a representative thermosetting bioelastomer known for its elasticity, biodegradability, and biocompatibility and is widely used in tissue engineering. However, the modification and drug loading of the PGS scaffold is still a key challenge due to its high temperature curing conditions and limited reactive groups, which seriously hinders its further functional application. Here, a simple versatile new strategy of super swelling-absorption and cross-linked networks locking is presented to successfully create the 3D printed PGS-CS/Gel scaffold for the first time based on FDA-approved PGS, gelatin (Gel) and chondroitin sulfate (CS). The PGS-CS/Gel scaffold exhibits the desirable synergistic properties of well-organized hierarchical structures, excellent elasticity, improved hydrophilicity, and cartilaginous bioactivity, which can promote the adhesion, proliferation, and migration of chondrocytes. Importantly, the rate of cartilage regeneration can be well-matched with degradation of PGS-CS/Gel scaffold, and achieve uniform and mature cartilage tissue without scaffold residual. The bioactive scaffold can successfully repair cartilage in a rabbit trochlear groove defect model indicating a promising prospect of clinical transformation.

Mechanically Robust and Room Temperature Self-Healing Ionogel Based on Ionic Liquid Inhibited Reversible Reaction of Disulfide Bonds.

Although highly desired, it is difficult to develop mechanically robust and room temperature self-healing ionic liquid-based gels (ionogels), which are very promising for next-generation stretchable electronic devices. Herein, it is discovered that the ionic liquid significantly reduces the reversible reaction rate of disulfide bonds without altering its thermodynamic equilibrium constant via small molecule model reaction and activation energy evolution of the dissociation of the dynamic network. This inhibitory effect would reduce the dissociated units in the dynamic polymeric network, beneficial for the strength of the ionogel. Furthermore, aromatic disulfide bonds with high reversibility are embedded in the polyurethane to endow the ionogel with superior room temperature self-healing performance. Isocyanates with an asymmetric alicyclic structure are chosen to provide optimal exchange efficiencies for the embedded disulfide bonds relative to aromatic and linear aliphatic. Carbonyl-rich poly(ethylene-glycol-adipate) diols are selected as soft segments to provide sufficient interaction sites for ionic liquids to endow the ionogel with high transparency, stretchability, and elasticity. Finally, a self-healing ionogel with a tensile strength of 1.65 ± 0.08 MPa is successfully developed, which is significantly higher than all the reported transparent room temperature self-healing ionogel and its application in a 3D printed stretchable numeric keyboard is exemplified.

Adaptable covalently cross-linked fibers.

Fibers, with over 100 million tons produced each year, have been widely used in various areas. Recent efforts have focused on improving mechanical properties and chemical resistance of fibers via covalent cross-linking. However, the covalently cross-linked polymers are usually insoluble and infusible, and thus fiber fabrication is difficult. Those reported require complex multiple-step preparation processes. Herein, we present a facile and effective strategy to prepare adaptable covalently cross-linked fibers by direct melt spinning of covalent adaptable networks (CANs). At processing temperature, dynamic covalent bonds are reversibly dissociated/associated and the CANs are temporarily disconnected to enable melt spinning; at the service temperature, the dynamic covalent bonds are frozen, and the CANs exhibit favorable structural stability. We demonstrate the efficiency of this strategy via dynamic oxime-urethane based CANs, and successfully prepare adaptable covalently cross-linked fibers with robust mechanical properties (maximum elongation of 2639%, tensile strength of 87.68 MPa, almost complete recovery from an elongation of 800%) and solvent resistance. Application of this technology is demonstrated by an organic solvent resistant and stretchable conductive fiber.

Nonadjacent Wireless Electrotherapy for Tissue Repair by a 3D-Printed Bioresorbable Fully Soft Triboelectric Nanogenerator.

Electrotherapy is a promising tissue repair technique. However, electrotherapy devices are frequently complex and must be placed adjacent to injured tissue, thereby limiting their clinical application. Here, we propose a general strategy to facilitate tissue repair by modulating endogenous electric fields with nonadjacent (approximately 44 mm) wireless electrotherapy through a 3D-printed entirely soft and bioresorbable triboelectric nanogenerator based stimulator, without any electrical accessories, which has biomimetic mechanical properties similar to those of soft tissue. In addition, the feasibility of using the stimulator to construct an electrical double layer with tissue for nonadjacent wireless electrotherapy was demonstrated by skin and muscle injury models. The treated groups showed significantly improved tissue repair compared with the control group. In conclusion, we developed a promising electrotherapy strategy and may inspire next-generation electrotherapy for tissue repair.

Chinese Tofu-Inspired Biomimetic Conductive and Transparent Fibers for Biomedical Applications.

Conductive fibers are vital for next-generation wearable and implantable electronics. However, the mismatch of mechanical, electrical, and biological properties between existing conductive fibers and human tissues significantly retards their further development. Here, the concept of neuro-like fibers to meet these aforementioned requirements is proposed. A new wet spinning process is established to continuously produce pure gelatin hydrogel fibers. The key is the controllable and rapid gelation of spinning solutions based on the salting-out effect, which is inspired by the Chinese food tofu. The resultant fibers exhibit neuro-like features of soft-while-strong mechanical properties, high ionic conductivity, and superior biological properties including biodegradability, biocompatibility, and edibility, which are crucial for implanted applications but seldom reported. Furthermore, all-weather suitable neuro-like fibers with excellent anti-freezing and water retention properties are developed by introducing glycerol for wearable applications. The optical fiber, transient electronics, and electronic data glove made of neuro-like fibers profoundly demonstrate their potential in biomedical applications.

Breathable, antifreezing, mechanically skin-like hydrogel textile wound dressings with dual antibacterial mechanisms.

Hydrogels are emerging as the most promising dressings due to their excellent biocompatibility, extracellular matrix mimicking structure, and drug loading ability. However, existing hydrogel dressings exhibit limited breathability, poor environmental adaptability, potential drug resistance, and limited drug options, which extremely restrict their therapeutic effect and working scenarios. Here, the current research introduces the first paradigm of hydrogel textile dressings based on novel gelatin glycerin hydrogel (glyhydrogel) fibers fabricated by the Hofmeister effect based wet spinning. Benefiting from the unique knitted structure, the textile dressing features excellent breathability (1800 times that of the commercially available 3 M dressing) and stretchability (535.51 ± 38.66%). Furthermore, the glyhydrogel textile dressing can also withstand the extreme temperature of -80 °C, showing the potential for application in subzero environments. Moreover, the introduction of glycerin endows the textile dressing with remarkable antibacterial property and expands the selection of loaded drugs (e.g., clindamycin). The prepared glyhydrogel textile dressing shows an excellent infected wound healing effect with a complete rat skin closure within 14 days. All these functions have not been achievable by traditional hydrogel dressings and provide a new approach for the development of hydrogel dressings.

Meniscus-Climbing System Inspired 3D Printed Fully Soft Robotics with Highly Flexible Three-Dimensional Locomotion at the Liquid-Air Interface.

Soft robotics locomotion at the liquid-air interface has become more and more important for an intelligent society. However, existing locomotion of soft robotics is limited to two dimensions. It remains a formidable challenge to realize three-dimensional locomotion (X, Y, and Z axes) at the liquid-air two-phase interface due to the unbalanced mechanical environment. Inspired by meniscus-climbing beetle larva Pyrrhalta, the mechanism of a three-phase (liquid-solid-air) contact line is here proposed to address the aforementioned challenge. A corresponding 3D printed fully soft robotics (named larvobot) based on photoresponsive liquid crystal elastomer/carbon nanotubes composites endowed repeatable programmable deformation and high degree-of-freedom locomotion. Three-dimensional locomotion at the liquid-air interface including twisting and rolling-up has been developed. The equation of motion is established by analyzing the mechanics along the solid-water surface of the larvobot. Meanwhile, ANSYS is used to calculate the stress distribution, which coincides with the speculation. Moreover, soft robotics is remotely driven by light in a precise spatiotemporal control, which provides a great advantage for applications. As an example, we demonstrate the controllable locomotion of the soft robotics inside closed tubes, which could be used for drug delivery and intelligent transportation.