The development of multifunctional films with rapidly killing microorganisms and adsorbing residual antibiotics in wastewater remains a challenging endeavor. In this work, the chitosan/zinc ion/polyoxometalate (CS/Zn 2+ /POM) multifunctional films were prepared by the freeze-drying method using chitosan, ZnO, and POM. Notably, the CS/Zn 2+ /POM films exhibited excellent bactericidal properties against Gram-positive/ negative bacterial strains including Staphylococcus aureus (S. aureus, 99.80%), Escherichia coli (E. coli, 99.82%), and drug-resistant E. coli bacterial strains (kanamycin-resistant E. coli, 87.76% and ampicillinresistant E. coli, 99.71%). This may be due to the chelation of Zn 2+ with CS disrupting the cell membrane and bringing POM into direct contact with bacteria, leading to bacterial death. In addition, the CS/Zn 2+ /POM films showed good adsorption performance to a tetracycline (TC) solution (adsorption rate 75.2%). Further studies showed that the main process of tetracycline removal by CS/Zn 2+ /POM films was controlled by a physical adsorption. This POM-based film material has an important potential for the synthesis of broad-spectrum antimicrobial materials for the removal of residual antibiotics from water pollutants such as tetracycline.