Polyvinyl Alcohol‐Based Thermogel with Tunable Gelation and Self‐Healing Property

Injectable thermogelated hydrogels with self‐healing and multi‐responsiveness are emerging as a class of significant “smart” materials because of their many potential applications. However, there are only very limited precedents that combine thermogels with self‐healing and tunable functions. In this work, it is demonstrated that N‐alkyl substituted carbamate modified polyvinyl alcohol with borax as a crosslinker enables a variety of tunable and dynamic thermogelation properties. As far as it is known, this is the first polyvinyl alcohol–based thermogel system. This system characterizes shear thinning, multiple responsiveness, and dynamic gelation features. Systematic investigation suggests that these features collaborate to contribute to attractive injectability, quick self‐healing ability, and tunable thermogelation behavior. A stepwise in situ gelation and carbon dioxide–triggered release are demonstrated. For the first time, N‐alkyl substituted carbamate modified polyvinyl alcohol with borax as a crosslinker enables a variety of tunable and dynamic thermogelation properties, including shear thinning, multiple responsiveness, dynamic gelation features and self‐healing. This system can be practically useful in the biorelevant fields.