Ultrafast and Multi‐Stimuli‐Responsive MXene Soft Actuators via Heterostructure Design for Biomimetic Applications

Abstract Multi‐stimulus‐responsive actuators demonstrate significant potential in the fields of bionic robots, flexible electronics, and smart sensing. However, their practical applications have been hindered by inadequate environmental stability, limited response modes, and insufficient mechanical durability. This study designs an MXene&PVA/CNT&PVA (MP/CP) bilayer film actuator that achieves high‐performance multi‐field‐coupled actuation through interfacial chemistry modulation and dynamic strain gradient synergy. The actuator demonstrates fast and multimodal responsiveness, achieving a bending deformation of 516° within 0.5 s (with full recovery in 1 s) at 90% relative humidity (RH), reaching an even larger bending angle of 1128° under near‐infrared (NIR) light stimulation (200 mW cm ^{− 2} ), while simultaneously exhibiting distinct sensitivity to polar solvents, and maintains exceptional environmental stability and cycling endurance. Capitalizing on these advantages, the MP/CP film enables precise control of smart switches, adaptive curtain operation, and biomimetic motions such as robotic locomotion and butterfly‐like multimodal flapping through sequential stimulus regulation. This work provides novel insights for developing multifunctional smart actuators, with broad application prospects in adaptive soft robotics and environmental interactive systems.