Nowadays, the rapid emergence of antibiotic-resistant pathogens has become a serious threat to human health. As an effective antimicrobial therapy, supramolecular materials show unprecedented advantages because of their flexible and adjustable interactions with biological molecules. Supramolecular hydrogels are now widely applied in biomedical fields because of their outstanding biocompatibility, high water content, easy preparation, and unique functions. Herein, we conveniently prepared a stable supramolecular hydrogel by simply mixing β-cyclodextrin-modified chitosan (CS-CD) with AgNO3 in a basic environment. The obtained supramolecular hydrogel, which is positively charged and possesses numerous β-cyclodextrin cavities, could efficiently load anionic drug diclofenac sodium (DS) through the electrostatic interaction and host-guest inclusion. Significantly, the biological experiments demonstrated that this supramolecular hydrogel exhibited a high antibacterial effect and good ability of promoting wound healing owing to the cooperative contribution of CS, Ag+, and DS.