One‐Pot Synthesis of Melt‐Processable Supramolecular Soft Actuators

The application of reprocessable and reprogrammable soft actuators is limited by the synthetic strategies, 3D‐shaping capabilities, and small deformations. In this work, melt‐processable supramolecular soft actuators based on segmented copolymers containing thiourethane and liquid crystal segments have been prepared via sequential thiol addition reactions in a one‐pot approach using commercially available building blocks. The actuators demonstrated immediate, reversible response and weightlifting capabilities with large deformations up to 32 %. Through exploiting the supramolecular cross‐links, the material could be recycled and reprogrammed into 3D actuators and welded into an actuator assembly with different deformation modes. Our work offers a one‐pot synthesis and straightforward melt‐processable approach to prepare supramolecular soft actuators with large deformations that can be reprocessed and reprogrammed into arbitrary 3D shapes.