With recent outbreaks of fatal strains of diseases and the emergency of antibiotic resistance, there is a pressing demand to discover bactericidal materials that can effectively reduce or prevent infections by pathogenic bacteria. Herein, silver(I) metal organic frameworks Ag2(HBTC) were embedded into biocompatible polylactic acid (PLA) fibrous membranes through an electrospinning process as an antibiotic-free material for effective bacterial killing. The as-synthesized Ag2(HBTC)/PLA composite membrane showed an inactivation efficiency of more than 99.9% against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) at a concentration of 200-250 mg L-1. Mechanistic investigation indicated that the steady release of Ag+ ions and ˙OH generation from the composites contributed to the efficient antibacterial activities through irreversible damage to the bacterial cell membranes. In-depth proteomic analysis demonstrated that Ag2(HBTC)/PLA exerted a biological effect towards bacterial cells through down-regulating functional proteins, thereby destroying the central biochemical pathways of the cellular energy metabolism process, reducing resistance to oxidative damage and inhibiting cell division. In general, this study shows a promising perspective on designing MOF/PLA membranes with broad-spectrum disinfection capability for potential environmental sterilization and public healthcare protection.