Particulate matter (PM) air pollution is becoming more and more serious and dangerous to public health, especially in developing countries where industrialization is accelerating. The use of electrospun membrane-based materials for air filtration is a widespread and effective way to help individuals avoid air pollution. However, most electrospun membrane preparation processes require the use of organic solvents, resulting in secondary environmental pollution. In this study, an environmentally friendly polyvinyl alcohol (PVA) - tannic acid (TA) composite nanofiber membrane filter was prepared by the green electrospinning and the physical cross-linking method. The filtration efficiency of the membrane filter for PM 1.0 reached 99.5%, and the pressure drop was only 35 Pa. In addition, due to the existence of intermolecular hydrogen bond between PVA and TA, the mechanical properties of the nanofiber membrane were improved to meet the requirements of practical application of the filter. Therefore, the PVA-TA composite nanofiber membrane is expected to provide a solution for the development of efficient and environmentally friendly air filter.