Designing multistimuli responsive soft actuators which can mimic advanced and sophisticated biological movements through simple configuration is highly demanded for the biomimetic robotics application. Here, inspired by the human's flick finger behavior which can release large force output, a soft jumping robot mimicking the gymnast's somersault is designed based on the rolled carbon nanotube/polymer bilayer composite actuator. This new type of rolled bilayer actuator with tubular shape is fabricated and shows electrically and sunlight‐induced actuation with remarkable performances including ultralarge deformation from tubular to flat (angel change >200° or curvature >2 cm−1), fast response (<5 s), and low actuation voltage (≤10 V). Besides jumping, the uniquely reversible rolling–unrolling actuation can lead to other smart soft robots with versatile complex biomimetic motions, including light‐induced tumbler with cyclic wobbling, electrically/light‐induced crawling‐type walking robots and grippers, electrically induced mouth movement, and ambient‐sunlight‐induced blooming of a biomimetic flower. These results open the way for using one simple type of actuator structure for the construction of various soft robots and devices toward practical biomimetic applications.

Soft actuators and microrobots that can move spontaneously and continuously without artificial energy supply and intervention have great potential in industrial, environmental, and military applications, but still remain a challenge. Here, a bioinspired MXene-based bimorph actuator with an asymmetric layered microstructure is reported, which can harness natural sunlight to achieve directional self-locomotion. We fabricate a freestanding MXene film with an increased and asymmetric layered microstructure through the graft of coupling agents into the MXene nanosheets. Owing to the excellent photothermal effect of MXene nanosheets, increased interlayer spacing favoring intercalation/deintercalation of water molecules and its caused reversible volume change, and the asymmetric microstructure, this film exhibits light-driven deformation with a macroscopic and fast response. Based on it, a soft bimorph actuator with ultrahigh response to solar energy is fabricated, showing natural sunlight-driven actuation with ultralarge amplitude and fast response (346°in 1 s). By utilizing continuous bending deformation of the bimorph actuator in response to the change of natural sunlight intensity and biomimetic design of an inchworm to rectify the repeated bending deformation, an inchwormlike soft robot is constructed, achieving directional self-locomotion without any artificial energy and control. Moreover, soft arms for lifting objects driven by natural sunlight and wearable smart ornaments that are combined with clothing and produce three-dimensional deformation under natural sunlight are also developed. These results provide a strategy for developing natural sunlight-driven soft actuators and reveal great application prospects of this photoactuator in sunlight-driven soft biomimetic robots, intelligent solar-energy-driven devices in space, and wearable clothing.

Mimicking the intelligence of biological organisms in artificial systems to design smart actuators that act autonomously in response to constant environmental stimuli is crucial to the construction of intelligent biomimetic robots and devices, but remains a great challenge. Here, a light-driven autonomous carbon-nanotube-based bimorph actuator is developed through an elaborate structural design. This curled droplet-shaped actuator can be simply driven by constant white light irradiation, self-propelled by a lightmechanical negative feedback loop created by light-driven actuation, time delay in the photothermal response along the actuator, and good elasticity from the curled structure, performing a continuously self-oscillating motion in a wavelike fashion, which mimics the human sit-up motion. Moreover, this autonomous self-oscillating motion can be further tuned by controlling the intensity and direction of the incident light. The autonomous actuator with continuous wavelike oscillating motion shows immense potential in light-driven biomimetic soft robots and optical-energy-harvesting devices. Furthermore, a self-locomotive artificial snake with phototaxis is constructed, which autonomously and continuously crawls toward the light source in a wave-propagating manner under constant light irradiation. This snake can be placed on a substrate made of triboelectric materials to realize continuous electric output when exposed to constant light illumination.

Developing self‐oscillating soft actuators that enable autonomous, continuous, and directional locomotion is significant in biomimetic soft robotics fields, but remains great challenging. Here, an untethered soft photoactuators based on covalently‐bridged black phosphorus‐carbon nanotubes heterostructure with self‐oscillation and phototactic locomotion under constant light irradiation is designed. Owing to the good photothermal effect of black phosphorus heterostructure and thermal deformation of the actuator components, the new actuator assembled by heterostructured black phosphorus, polymer and paper produces light‐driven reversible deformation with fast and large response. By using this actuator as mechanical power and designing a robot configuration with self‐feedback loop to generate self‐oscillation, an inchworm‐like actuator that can crawl autonomously towards the light source is constructed. Moreover, due to the anisotropy and tailorability of the actuator, an artificial crab robot that can simulate the sideways locomotion of crabs and simultaneously change color under light irradiation is also realized.

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