Constructing Shape Memory Polymer Based on the Synergy of Topologically Interlocked Slide‐Ring Structure and Dynamic Disulfide Bonds

ABSTRACT Shape memory polymers (SMPs) face a critical challenge in designing novel network architectures that fundamentally regulate intermolecular chain interactions while simultaneously achieving high shape fixation/recovery rates. Herein, we report a dual dynamic covalent shape memory polymer (DDC‐SMP) that synergistically integrates slide‐ring (SR) cross‐links and dynamic disulfide (S–S) bonds. The SR structure enhances chain mobility by sliding motion, while the S–S bonds enable network reconfiguration through reversible exchange. This synergy endows the DDC‐SMP with exceptional shape memory properties, including high shape fixation (> 97%) and recovery rates (> 97%), and excellent cyclic stability (retaining > 96% performance after three cycles at 50% and 200% strain). This dual dynamic bonding strategy establishes a new paradigm for constructing advanced polymer networks, laying the foundation for high‐performance shape memory materials.