Bioactive hydrogels self-assembled from naturally occurring
herbal
small molecules are attracting growing interest for applications in
wound healing, due to their versatile intrinsic biological activities,
excellent biocompatibility, as well as facile, sustainable, and eco-friendly
processes. However, the development of supramolecular herb hydrogels
with sufficient strength and multifunctionality as an ideal wound
dressing in clinical practice remains a challenge. In this work, inspired
by the efficient clinic therapy and directed self-assembly of natural
saponin glycyrrhizic acid (GA), we create a novel GA-based hybrid
hydrogel to promote full-thickness wound healing and bacterial-infected
wound healing. This hydrogel possesses excellent stability and mechanical
performance and multifunctional properties, including injectable,
shape-adaptation and remodeling, self-healing, and adhesive abilities.
This is attributed to the hierarchical dual-network that comprises
the self-assembled hydrogen-bond fibrillar network of aldehyde-contained
GA (AGA) and the dynamic covalent network through Schiff base reaction
between AGA and a biopolymer carboxymethyl chitosan (CMC). Notably,
benefiting from the inherent strong biological activity of GA, the
AGA-CMC hybrid hydrogel exhibits unique and significant anti-inflammation
effects and antibacterial ability, especially toward the Gram-positive Staphylococcus aureus (S. aureus). In vivo
experiments demonstrate that the AGA-CMC hydrogel promotes uninfected
skin wound healing and S. aureus-infected skin wound
healing by enhancing the formation of granulation tissue, facilitating
collagen deposition, reducing bacterial infection, and downregulating
inflammatory response. This study highlights the design of new and
multifunctional bioactive herb hydrogels from natural drug-food homologous
small molecules, which can serve as a promising wound-healing dressing
for biomedical applications.