Ultrafast Bi‐Directional Bending Moisture‐Responsive Soft Actuators through Superfine Silk Rod Modified Bio‐Mimicking Hierarchical Layered Structure

Abstract Development of stimulus‐responsive materials is crucial for novel soft actuators. Among these actuators, the moisture‐responsive actuators are known for their accessibility, eco‐friendliness, and robust regenerative attributes. A major challenge of moisture‐responsive soft actuators (MRSAs) is achieving significant bending curvature within short response times. Many plants naturally perform large deformation through a layered hierarchical structure in response to moisture stimuli. Drawing inspiration from the bionic structure of Delosperma nakurense (D. nakurense) seed capsule, here the fabrication of an ultrafast bi‐directional bending MRSAs is reported. Combining a superfine silk fibroin rod (SFR) modified graphene oxide (GO) moisture‐responsive layer with a moisture‐inert layer of reduced graphene oxide (RGO), this actuator demonstrated large bi‐directional bending deformation (−4.06 ± 0.09 to 10.44 ± 0.00 cm −1 ) and ultrafast bending rates (7.06 cm −1 s −1 ). The high deformation rate is achieved by incorporating the SFR into the moisture‐responsive layers, facilitating rapid water transmission within the interlayer structure. The complex yet predictable deformations of this actuator are demonstrated that can be utilized in smart switch, robotic arms, and walking device. The proposed SFR modification method is simple and versatile, enhancing the functionality of hierarchical layered actuators. It holds the potential to advance intelligent soft robots for application in confined environments.