ABSTRACT Multimodal reversible deformation is crucial for soft robots and intelligent actuators due to its adaptability to complex environments. The inherent programmability and reversible actuation capabilities of two‐way shape memory polymers make them ideal materials for achieving this functionality. However, the reliance on external force‐assisted programming inherently limits the realization of this feature. Here, we developed a controllable crosslinking gradient polyester (CGPES) by a solvent evaporation‐assisted photocrosslinking strategy. The cross‐linking gradient constitutes an internal asymmetry, enabling a single material to exhibit multimodal/fully autonomous reversible shape memory deformation, such as reversible pendulum and bow‐shaped bending under tensile programming, gravity‐driven self‐programming, and reversible torsional bending. Furthermore, CGPES also has photothermal response characteristics, demonstrating remote control grasp‐release and complex deformation driving capabilities. This work provides a new strategy for constructing multimodal/fully autonomous two‐way shape memory polymers, demonstrating significant potential for intelligent actuators and soft robots.
Guo et al. (Fri,) studied this question.