Cyclodextrin-polypseudorotaxane hydrogels have attracted extensive attention for their potential application in biomedical fields. Herein, we develop a facile strategy for the in situ formation of mechanically tough polypseudorotaxane hydrogels through photoinitiated copolymerization of poly(ethylene glycol) methyl ether methacrylate, acrylamide and sodium acrylate in α-CD solution at 60 °C. For the first time, we manage to screen the host-guest interaction between α-CD and PEG before copolymerization in the presence of a temporary hydrogen bonding weakening monomer (acrylamide) at a suitable temperature (60 °C). This shielding effect weakens gradually during polymerization, thus leading to the formation of polypseudorotaxane aggregations and a tough physical hydrogel. The hydrogel can bear a large compressive strain (80%) without rupture, and exhibits excellent antifatigue properties. Furthermore, this hydrogel could be endowed with thermal/ascorbic acid activated shape memory performance after being treated with FeCl solution. This simple method will contribute to the design and application of smart supramolecular hydrogels.
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