Bacterial infection has always been a great threat to public health, and new antimicrobials to combat it are urgently needed. Here, a series of quaternized β-chitin derivatives is prepared simply and homogeneously in an aqueous KOH/urea solution, which is a high-efficiency, energy-saving, and "green" route for the modification of chitin. The mild reaction conditions keep the acetamido groups of β-chitin intact and introduce quaternary ammonium groups on the primary hydroxyl at the C-6 position of the chitin backbone, allowing the quaternized β-chitin derivatives (QCs) to easily form micelles. These QCs are found to exhibit excellent antimicrobial activities against Escherichia coli, Staphylococcus aureus, Candida albicans, and Rhizopus oryzae with minimum inhibitory concentrations (MICs) of 8, 12, 60, and 40 µg mL , respectively. As a specific highlight, their inherent outstanding biocompatibility and significant accelerating effects on the healing of uninfected, E. coli-infected, and S. aureus-infected wounds imply that these novel polysaccharide-based materials can be used as dressings for clinical skin regeneration, particularly for infected wounds.