Injectable and self‐healing dual crosslinked gelatin/kappa‐carrageenan methacryloyl hybrid hydrogels via host‐guest supramolecular interaction for wound healing

Injectable hydrogels based on natural polymers have shown great potential for various tissue engineering applications, such as wound healing. However, poor mechanical properties and weak self-healing ability are still major challenges. In this work, we introduce a host-guest (HG) supramolecular interaction between acrylate-β-cyclodextrin (Ac-β-CD) conjugated on methacrylated kappa-carrageenan (MA-κ-CA) and aromatic residues on gelatin to provide self-healing characteristics. We synthesize an MA-κ-CA to conjugate Ac-β-CD and fabricate dual crosslinked hybrid hydrogels with gelatin to mimic the native extracellular matrix (ECM). The dual crosslinking occurs on the MA-κ-CA backbone through the addition of KCl and photocrosslinking process, which enhances mechanical strength and stability. The hybrid hydrogels exhibit shear-thinning, self-healing, and injectable behavior, which apply easily under a minimally invasive manner and contribute to shear stress during the injection. In-vitro studies indicate enhanced cell viability. Furthermore, scratch assays are performed to examine cell migration and cell-cell interaction. It is envisioned that the combination of self-healing and injectable dual crosslinked hybrid hydrogels with HG interactions display a promising and functional biomaterial platform for wound healing applications.