A Rapidly Self‐Healing Host–Guest Supramolecular Hydrogel with High Mechanical Strength and Excellent Biocompatibility

It is still a challenge to achieve both excellent mechanical strength and biocompatibility in hydrogels. In this study, we exploited two interactions to form a novel biocompatible, slicing-resistant, and self-healing hydrogel. The first was molecular host-guest recognition between a host (isocyanatoethyl acrylate modified β-cyclodextrin) and a guest (2-(2-(2-(2-(adamantyl-1-oxy)ethoxy)ethoxy)ethoxy)ethanol acrylate) to form "three-arm" host-guest supramolecules (HGSMs), and the second was covalent bonding between HGSMs (achieved by UV-initiated polymerization) to form strong cross-links in the hydrogel. The host-guest interaction enabled the hydrogel to rapidly self-heal. When it was cut, fresh surfaces were formed with dangling host and guest molecules (due to the breaking of host-guest recognition), which rapidly recognized each other again to heal the hydrogel by recombination of the cut surfaces. The smart hydrogels hold promise for use as biomaterials for soft-tissue repair.