Air pollution by particulate matter (PM) and airborne pathogens causes severe health problems in the human body. Presently, popular disposable air filters yield huge waste and have a fatal impact on the environment. Postuse cleaning of air filters also leads to secondary air and water pollution. Here, we report a sunlight-driven self-cleaning PM filter by coupling a full-solar-spectrum-active photocatalyst comprising up-conversion nanoparticles (UCNPs) decorated with semiconductor iron(III) oxide (UCNP@α-Fe2O3) shells stabilized upon graphene functionalized borosilicate fibrous membrane (rGO-BF). While rGO-BF ensures high PM adsorption, UCNP@α-Fe2O3 (NP) enables self-photodegradation of adsorbed PM under abundant sunlight and subsequent membrane regeneration, while preventing secondary air or water pollution. Rational surface chemistry and optimal microstructure enable our filters to remove >99% of PM2.5 under deplorable air-quality conditions. Moreover, our filter shows excellent antibacterial activity toward E. coli and S. aureus, demonstrating its potential for practical utilization in face masks, air filtering devices, and protective medical wear. This work successfully suggests an intriguing design platform for self-sustainable zero-waste air filter membranes.