Synergistic Covalent and Supramolecular Polymer Networks Enabled by Unsymmetrical Topological Nodes

Achieving efficient synergy between covalent and supramolecular polymers is an effective strategy for developing novel polymeric materials. However, realizing this synergy through rational chemical design to efficiently integrate both types of polymers within a single polymer network remains a significant challenge. Here, we achieve efficient synergy between covalent and supramolecular polymer chains by inducing entanglement of unsymmetrical topological nodes. Benefiting from the molecular entanglement strategy, this synergistic network effectively integrates the stability of a covalent polymer and the dynamics of a supramolecular polymer. While maintaining the integrity of the network, the reversible host-guest recognition in the supramolecular polymer dissipates the applied energy, thus allowing the mechanical properties of the entire network to be regulated. Besides, the host-guest recognition pairs can serve as splicing points for integrating additional polymers, transforming the topologically entangled covalent-supramolecular synergistic polymer platform into a multifunctional platform that accommodates a variety of polymers, significantly increasing the diversity of their structures and properties. These findings may spur further innovations in the field of polymers in general, as well as promote a deeper understanding of dynamic chemistry.