Injectable, self-healable and antibacterial multi-responsive tunicate cellulose nanocrystals strengthened supramolecular hydrogels for wound dressings

Wound dressing with an improved structural and functional recapitulation of damaged organs, efficient self-healing and antibacterial properties that can well integrate with tissue are urgently needed in wound management. Supramolecular hydrogels confer control over structural properties in a reversible, dynamic and biomimetic fashion. Herein, a kind of injectable, self-healing and antibacterial supramolecular hydrogel with multi-responses were fabricated by mixing phenylazo-terminated Pluronic F127, quaternized chitosan-graft-cyclodextrin and polydopamine coated tunicate cellulose nanocrystals under physiological conditions. By exploiting the photoisomerization of azobenzene under different wavelengths, a supramolecular hydrogel featuring a changing crosslink density of network was obtained. The corporation of polydopamine coated tunicate cellulose nanocrystals strengthens the hydrogel network with Schiff base bonds and hydrogen bonds, which avoids complete gel-sol transition. The inherent antibacterial property, drug release behavior, self-healing ability, hemostatic performance and biocompatibility were investigated to confirm superiority in wound healing. Moreover, the curcumin loaded hydrogel (Cur-hydrogel) showed multi-responsive release profiles (light, pH, and temperature). A full-thickness skin defect model was built to confirm that Cur-hydrogels significantly accelerated wound healing rate with better granulation tissue thickness and collagen disposition. Overall, the novel photo-responsive hydrogel with coherent antibacterial property has great potential in the healthcare of wound healing. •Multifunctional supramolecular hydrogels with high mechanical strength were prepared.•Excellent multi-responsive controlled drug release, biocompatibility and wound healing performance were obtained.•Optimized supramolecular hydrogels can be used as wound dressing.