Injectable, remoldable hydrogels with thermoresponsiveness, self-healing and cytocompatibility constructed via orthogonal assembly of well-defined star and linear polymers

Thermoresponsive hydrogels, as a type of intelligent materials, have great potential for applications in the biomedical field. However, it is still a great challenge to develop hydrogels with regularly arranged networks and combination of high intelligence, multifunction, and good biocompatibility. Herein, we present a new family of supramolecular hydrogels constructed through the orthogonal assembly of well-defined star and linear polymer units. These units were synthesized by combining atom transfer radical polymerization (ATRP) and click reaction. The obtained hydrogels are injectable, processable and cytocompatible with thermoresponsiveness and self-healing properties. This work demonstrates the great potential of reticular design and orthogonal host-guest assembly towards the creation of highly-intelligent and multifunctional hydrogel materials.