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Synergistic covalent-and-supramolecular polymers, in which covalent polymers and supramolecular polymers connect with each other through [2]pseudorotaxane moieties, are designed and synthesized. The unique topological structure effectively enhances the synergistic effect between these two polymers, thereby generating a novel class of mechanically adaptive materials.A series of alkoxylated isobenzofuranones were conveniently synthesized from the reaction of 2-(1-arylvinyl)benzoic acids with PhI(OR)2, generated in situ from the reaction of