Topological Integration of Slide‐Ring and Entangled Networks

ABSTRACT Topological regulation of polymer networks has emerged as an effective strategy for enhancing the mechanical performance of elastomeric materials. Among various topological architectures, slide‐ring networks and entangled networks have attracted considerable attention, owing to their unique dynamic mobility and spatial interlocked effects, respectively. However, these two topological motifs have so far been explored separately, and their synergistic integration within a single elastomer network remains a significant challenge. Herein, we construct a synergistic topological elastomeric network ( SEPN ) by integrating slide‐ring and entangled structures through a molecular‐level interpenetration−polymerization co‐evolution process, followed by aldimine crosslinking and metal‐coordination assembly. The resulting network combines the dynamic mobility of slide‐ring structures with the spatial interlocked effect of entangled nodes, enabling efficient stress redistribution and energy dissipation. Consequently, SEPN exhibits an exceptional combination of high strength (24.3 MPa), superior toughness (327 MJ/m 3 ), large extensibility (2540%), and dynamic mechanical adaptability. This work establishes a topological synergy strategy for designing next‐generation high‐performance elastomeric materials.