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Abstract The emergence of the SARS‐CoV‐2 pandemic and airborne particulate matter (PM) pollution has led to remarkably high demand for face masks. However, conventional respirators are intended for single use and made from nondegradable materials, causing serious concern for a plastic‐waste environmental crisis. Furthermore, these facemasks are weakened in humid conditions and difficult to decontaminate. Herein, a reusable, self‐sustaining, highly effective, and humidity‐resistant air filtration membrane with excellent particle‐removal efficiency is reported, based on highly controllable and stable piezoelectric electrospun poly (l‐lactic acid) (PLLA) nanofibers. The PLLA filter possesses a high filtration efficiency (>99% for PM 2.5 and>91% for PM 1.0) while providing a favorable pressure drop (≈91 Pa at normal breathing rate) for human breathing due to the piezoelectric charge naturally activated by respiration through the mask. The filter has a long, stable filtration performance and good humidity resistance, demonstrated by a minimal declination in the filtration performance of the nanofiber membrane after moisture exposure. The PLLA filter is reusable via common sterilization tools (i.e., an ultrasonic cleaning bath, autoclave, or microwave). Moreover, a prototype of a completely biodegradable PLLA nanofiber‐based facemask is fabricated and shown to decompose within 5 weeks in an accelerated degradation environment.