Ultra‐Large Stress and Strain Polymer Nanocomposite Actuators Incorporating a Mutually‐Interpenetrated, Collective‐Deformation Carbon Nanotube Network

Abstract Stimulus‐responsive polymer‐based actuators are extensively studied, with the challenging goal of achieving comprehensive performance metrics that include large output stress and strain, fast response, and versatile actuation modes. The design and fabrication of nanocomposites offer a promising route to integrate the advantages of both polymers and nanoscale fillers, thus ensuring superior performance. Here, it is started from a three‐dimensional (3D) porous sponge to fabricate a mutually interpenetrated nanocomposite, in which the embedded carbon nanotube (CNT) network undergoes collective deformation with the shape memory polymer (SMP) matrix during large‐degree stretching and releasing, increases junction density with polymer chains and enhances molecular orientation. These features result in substantial improvement of the overall mechanical properties and during thermally actuated contraction, the bulk SMP/CNT composites exhibit output stresses up to 19.5 ± 0.97 MPa and strains up to 69%, accompanied by a rapid response and high energy density, exceeding the majority of recent reports. Furthermore, electrical actuation is also demonstrated via uniform Joule heating across the self‐percolated CNT network. Applications such as low‐temperature thermal actuated vascular stent and wound dressing are explored. These findings lay out a universal blueprint for developing robust and highly deformable SMP/CNT nanocomposite actuators with broad potential applications.