Environmentally friendly food packaging currently attracts much interest. Sodium trimetaphosphate (STMP) finds specialized applications in food, but it is rarely used as a crosslinking agent. In this study, STMP was used as a crosslinking agent to prepare chitosan/methylcellulose composite films. Both antibacterial and physicochemical properties of the composite film were improved by crosslinking with STMP. The crosslinked films, with good antibacterial activity (~99%), had increased tensile strength, a higher elongation at break, a lower swelling ratio and solubility, and a lower enzymatic degradation than the non-crosslinked films. Furthermore, the crosslinked films showed an excellent preservative effect on fresh-cut wax gourd after three days at room temperature. The obtained films crosslinked by STMP can be potentially applied to the food industry, such as food functional packaging, providing a novel alternative to traditional plastic packages.