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.

Designing artificial muscle actuators with diversely complex deformation and multifunction is crucial to the soft robots and their bioinspired applications. Herein, by combing the hygroexpansion and thermal expansion commonly existed in nature, electrically driven paper‐based bilayer actuator is fabricated by a simple printing method. This actuator exhibits large (270°) and anisotropic deformation coupled with features of low‐cost, superior stability, and additional reversible color‐change function. More importantly, the tailoring and heat setting are used to further design the actuator shape, thus obtain multiform deformation (bending, elongation, and folding), and more complicated deformation similar to the arm motion. Based on these actuators, variously bioinspired motions can be constructed. Inspired by the structure of the crystalline lens and ciliary muscle in human eyeball, a biomimetic lens which can change the focal length under electrical stimulation is fabricated. Moreover, W‐shaped robotic arm for manipulating microliquid in 3D direction and catapulting the object into air, in‐pipe spiral robotic arm for pushing objects out of the pipe, and artificial snake capable of deformation and color‐change simultaneously, are also fabricated. This paper‐based actuator together with bioinspired design may open new perspective on the multifunctional smart robots and biomimetic devices.

A multi-functional wearable sensor mimicking human skin is constructed based on an asymmetric graphene composite film, showing sensing and light-induced actuation.