Multi‐Functional Supramolecular‐Polymeric Hybrid Hydrogel for Promoting Cutaneous Wound Repair†

Comprehensive Summary Supramolecular‐polymeric hybrid hydrogels combining advantages of the assembled supramolecular networks and polymeric networks have attracted considerable attention recently. However, they are rarely used as multi‐functional wound dressing materials. In this work, we report a supramolecular‐polymeric hybrid hydrogel consisting of a co‐assembled DBS‐COOH/Naproxen network (DBS/NAP) and a polymeric gelatin (G)/quaternary ammonium group (Q) and phenylboronic acid groups (PBA)‐grafted chitosan (QCS‐PBA) network (G/QCS) for accelerating skin wound healing. The polymeric networks could obviously enhance the mechanical properties of the drug‐derived supramolecular networks. Q groups endowed the hydrogel with enhanced antibacterial properties. Borate ester crosslinking between PBA groups and diol groups in DBS‐COOH could effectively scavenge reactive radicals. The hybrid hydrogel exhibited tunable mechanical and adhesive properties due to the temperature‐responsive gelatin networks. NAP could gradually release from hybrid hydrogel networks thus continuously relieving inflammation. Finally, the biocompatible, adhesive, antibacterial and antioxidant hybrid G/QCS‐DBS/NAP gel could promote the in vivo healing stages in a full‐thickness wounds with increased collagen deposition, upregulated CD31 expression and down‐regulated TNF‐α expression. Overall, this multi‐functional supramolecular‐polymeric hybrid hydrogel exhibited great potential for treating skin defects as promising wound dressing materials.