Wet‐Spinning Carbon Nanotube/Shape Memory Polymer Composite Fibers with High Actuation Stress and Predesigned Shape Change

Abstract Actuators based on shape memory polymers and composites incorporating nanomaterial additives have been extensively studied; achieving both high output stress and precise shape change by low‐cost, scalable methods is a long‐term‐desired yet challenging task. Here, conventional polymers (polyurea) and carbon nanotube (CNT) fillers are combined to fabricate reinforced composite fibers with exceptional actuation performance, by a wet‐spinning method amenable for continuous production. It is found that a thermal‐induced shrinkage step could obtain densified strong fibers, and the presence of CNTs effectively promotes the tensile orientation of polymer molecular chains, leading to much improved mechanical properties. Consequently, the CNT/ polyurea composite fibers exhibit stresses as high as 33 MPa within 0.36 s during thermal actuation, and stresses up to 22 MPa upon electrical stimulation enabled by the built‐in conductive CNT networks. Utilizing the flexible thin fibers, various shape change behavior are also demonstrated including the conversion between different structures/curvatures, and recovery of predefined simple patterns. This high‐performance composite fibers, capable of both thermal and electrical actuation and produced by low‐cost materials and fabrication process, may find many potential applications in wearable devices, robotics, and biomedical areas.