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Abstract: There is a consensus that the prevention of wound infection should be achieved in the following ways: (1) closing the wound to protect it from extra infection; (2) an antibacterial agent that could kill endogenous bacteria. However, existing bulk two-dimensional antibacterial materials show inefcient adhesion to wounds with complex morphology and thus cause the prevention of wound closure. Reducing the thickness of bulk two-dimensional materials to less than 100 nanometres endows them with great fexibility, which could allow them to adhere to wounds with complex morphology by only physical adhesion. Herein, a broad-spectrum and efcient antimicrobial peptide (AMP) was introduced to biocompatible methacrylated gelatine (GelMA) with multiple modifcation sites, which served as an inner antibacterial layer. After being combined with a biodegradable and good mechanical poly-l-lactide (PLLA) outer layer through plasma-treatment-assisted spin coating, we fnally constructed bilayered antibacterial nanosheets with a thickness of approximately 80 nm. These bilayered nanosheets possess good adhesion to surfaces with complex topography and thus achieve better wound closure than other bulk two-dimensional materials. Moreover, this AMP-grafted conjugation shows minimal cytotoxicity compared with Ag+ antibacterial agents, and the antibacterial rate of nanosheets is dependent on the graft rate of AMP. We suggest that this bilayered antibacterial nanosheet might be an advanced anti-infection dressing for wound treatment in clinical settings.