Here, a multifunctional poly (lactic acid)/copper-based metal–organic framework (PLA/CuMOF) degradablecomposite membrane featuring superior antibacterial and self-cleaning properties was fabricated viaa simple electrospinning process for high- efficiency filtration/separation. Benefiting from the decrease offiber diameter, the improved surface roughness and the surface charge of CuMOF, PLA/CuMOF fibrousmembrane achieved excellent capture ability for ultra-fine particles and superb purification capabilityfor real PM2.5 smoke. The differences of filtration capacity between PLA membrane and PLA/CuMOF membranewas further explored using analogue simulation with dynamic particle capture and airflow fielddistribution. Impressively, PLA/CuMOF fibrous membrane combines robust self-cleaning ability, effectiveantibacterial effect, and thermal management capability. Moreover, owing to the special selective wettabilityand chemical stability, PLA/CuMOF membrane possessed the stable oil–water separation performanceunder harsh environment (e.g., high acid, alkali, and salt). This degradable multifunctionalfiltration/separation fibrous membrane emerges a broad application prospect ranging from environmentalgovernance, industrial security to personal protection.