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In this study, chitosan was used to enhance the photodynamic antibacterial effect of curcumin through ionic interactions, and the antibacterial mechanism of this coating against Staphylococcus aureus at the cellular level was clarified from the aspects of morphological characteristics, cell membrane function, energy metabolism, and DNA structure. The results showed that chitosan significantly improve the antibacterial effect. The number of S. aureus decreased by 6.89 (lg(CFU/mL)) after the coating solution containing 15 mg/L curcumin was exposed to 420 nm blue light for 5 min. Curcumin concentration and illumination time were the major factors affecting the antibacterial effect of this technique. The photodynamic inactivation treatment produced highly oxidizing reactive oxygen species (ROS), damaging the cell membrane and increasing membrane permeability, thus leading to the leakage of cell contents and cell shrinkage. It also led to an increase in intracellular ROS levels, which disrupted the structure of endogenous enzymes to trigger the breakdown of the bacterial defense system and the oxidative decomposition of macromolecules such as DNA and proteins, eventually causing the death of S. aureus. Therefore, chitosan/curcumin photodynamic coating has application potential in controlling foodborne pollution of S. aureus.