Programmable and Multi‐Responsive Actuators with Reversible Deformation Based on Al/CNTs‐PDMS/SiOx Composite Films for Bionic Applications and Energy Harvesting

Abstract Bionic soft actuators have garnered considerable interest due to their promising applications in the realms of soft robotics, smart devices, and healthcare. Despite this, the capability for bi‐directional reversible deformation remains a rare feature among soft actuators. This study introduces a novel bidirectional reversible soft actuator comprised of a composite of multi‐walled carbon nanotubes‐polydimethylsiloxane (CNTs‐PDMS), silicon oxide (SiOx), and aluminum (Al). This composite is engineered through UV‐ozone surface modification and patterned deposition techniques. The actuator demonstrates superior programmable shape deformation capabilities, responding swiftly to stimuli from ethanol, other organic solvents, and near‐infrared (NIR) light. Furthermore, the actuator accomplishes a bidirectional reversible deformation process characterized by a “deformation‐anti‐deformation‐deformation” cycle when exposed to ethanol and organic solvents. The innovative structural design incorporating carbon isomers facilitates permits the direct observation of carbon materials’ molecular dynamics through macroscopic mechanical behaviors. The actuator's applications have been successfully demonstrated in flexible switches, bionic grasping, and bionic moth models. Additionally, in this study, the multilayer composite is integrated with perfluoroethylene propylene (FEP) to develop a liquid–solid triboelectric nanogenerator. This nanogenerator is capable of harvesting energy from water droplet impacts and powering an alcohol sensor, thereby establishing a self‐powered sensing system for monitoring alcohol volatilization.