Energy captured directly from sunlight provides an attractive approach towards fulfilling the need for green energy resources on the terawatt scale with minimal environmental impact. Collecting and storing solar energy into fuel through photocatalyzed water splitting to generate hydrogen in a cost-effective way is desirable. To achieve this goal, low cost and environmentally benign urea was used to synthesize the metal-free photocatalyst graphitic carbon nitride (g-C₃N₄). A porous structure is achieved via one-step polymerization of the single precursor. The porous structure with increased BET surface area and pore volume shows a much higher hydrogen production rate under simulated sunlight irradiation than thiourea-derived and dicyanamide-derived g-C₃N₄. The presence of an oxygen atom is presumed to play a key role in adjusting the textural properties. Further improvement of the photocatalytic function can be expected with after-treatment due to its rich chemistry in functionalization.

A photoactuator based on a tubular-shaped graphene composite bimorph is fabricated and shows reversible photoactuation with fast response and large deformation (deformation angle of ca. 479° in only 3.6 s), which is mostly attributed to the interfacial thermal stress. Various photoactuator devices based on the tubular bimorph, including a smart box and crawler-type robot that can mimic tank-track motion, are designed.

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.