Effective treatment of infectious keratitisn ecessitates a dual strategy to both eliminate pathogens and reduce inflammation. Nanozymes have emerged as promising tools in antimicrobial therapy due to their catalytic versatility. Graphdiyne (GDY) nanozymes are particularly important for their peroxidase-like (POD) activity and their ability to function as two-dimensional, layered porous nanocarriers. In this study, N,N'-di-sec-butyl-N,N'dinitroso-1,4-phenylenediamine (BNN6)-modified black phosphorus/graphdiyne (BP/GDY-BNN6) nanozymes are developed for the synergistic treatment of infectious keratitis. BP, with its photothermal and photodynamic properties, further contributes to antibacterial and anti-inflammatory effects. GDY not only functions as a nonmetallic nanozyme with catalytic activity, but also acts as a protective layer to enhance the stability of BP, thereby ensuring this nanoplatform highly suitable for the treatment of keratitis. Initially, the POD-like activity of GDY facilitates the production of center dot OH, effectively eliminating bacteria. The incorporation of BP introduces both photothermal and photodynamic properties, leading to the generation of heat and additional ROS. The photothermal effect further enables the controlled release of NO from BNN6, which synergizes with ROS to form peroxynitrite (ONOO-), enhancing the antimicrobial effect. Simultaneously, the residual NO targets inflammation at the corneal site, inhibiting inflammatory effects. BP/GDY-BNN6 nanozymes effectively trigger bacterial apoptosis without leading to cytotoxicity, or hemolytic activity, highlighting their excellent biocompatibility. In a bacterial keratitis model, BP/GDY-BNN6 nanozymes demonstrate significant antibacterial and antiinflammatory effects under 808 nm NIR alone, without exogenous H2O2. The synergistic action of photothermal, photodynamic, and NO-releasing properties under NIR illumination highlight the therapeutic potential of BP/GDY-BNN6 nanozymes for treating infectious keratitis.