Toward a versatile toolbox for cucurbit[n]uril‐based supramolecular hydrogel networks through in situ polymerization

The success of exploiting cucurbit[n]uril (CB[n])‐based molecular recognition in self‐assembled systems has sparked a tremendous interest in polymer and materials chemistry. In this study, polymerization in the presence of host‐guest complexes is applied as a modular synthetic approach toward a diverse set of CB[8]‐based supramolecular hydrogels with desirable properties, such as mechanical strength, toughness, energy dissipation, self‐healing, and shear‐thinning. A range of vinyl monomers, including acrylamide‐, acrylate‐, and imidazolium‐based hydrophilic monomers, could be easily incorporated as the polymer backbones, leading to a library of CB[8] hydrogel networks. This versatile strategy explores new horizons for the construction of supramolecular hydrogel networks and materials with emergent properties in wearable and self‐healable electronic devices, sensors, and structural biomaterials.