Highlight • Loading single/multilayer, uncharged/charged nanofiber filter experiments. • Charged/electret multilayer nanofiber filter increases greatly aerosol capacity. • Electret 4-layer nanofiber filter >50% more capacity than 1-layer uncharged nanofiber filter. • Filter fully utilized from charged fibers, 4X aerosols captured in depth filtration. • Lowest possible pressure gradient 11 Pa/gsm deposit., Aerosol loading behavior of PVDF nanofiber electret filters using neutrally charged nano- and submicron aerosols was investigated experimentally for the first time. The loading behavior include variations of filtration efficiency and pressure drop and distribution of deposited aerosols in the filters all having the same fiber basis weight (3.060 gsm). Through the filtration efficiency variations of uncharged/charged, single-/multi-layer filters with aerosol loading, it was observed that mechanical PVDF filters had continuously increasing filtration efficiency, while PVDF electret filters had initially decreasing and subsequently increasing filtration efficiency until reaching 100% due to diminishing electrostatic effect and enhancing mechanical effect. By combining the pressure drop evolution of different filters during aerosol loading and detailed SEM images of the loaded filters, we have demonstrated that multilayer PVDF filters, especially the electret ones, could significantly slow down the pace of filter clogging (skin effect) and increase significantly the aerosol holding capacity during depth filtration. Generally, the multilayer nanofiber filters received the most aerosol deposit during depth filtration, whereas the single-layer nanofiber filters with the same basis weight of fibers received the most deposit during cake filtration. The multilayer nanofiber filters had approximately 70% aerosol deposit in the filter during depth filtration fully utilizing the full filter thickness, especially for the electret filters that had charged fibers, and only 30% deposit in the cake. On the contrary, the single-layer uncharged/charged nanofiber filters were exactly the reverse due to persistency of the skin effect with only 30% deposit in the filter mostly located in the upstream layer, yet 70% deposit in the cake. During depth filtration, the pressure drop per added mass deposit for the multilayer electret filter was very low at 11 Pa gsm−1, which was at least twice below any other nanofiber filters. This was all attributed to the uniform capture of aerosols by electrostatic effect across the entire filter depth from the upstream to downstream layers of the multilayer electret filter. The above conclusion was confirmed by the detailed SEM images taken across the different filter layers for the multilayer filter configuration. The 4-layer electret nanofiber filter with a 3.060-gsm basis weight has 4 times more aerosol holding capacity than the single uncharged/charged nanofiber filter with the same fiber basis weight in depth filtration. Based on the standpoint of highest efficiency and capacity with maximum pressure drop 800 Pa imposed on the filtration operation, the 4-layer nanofiber electret was the best among all 4 filters. It had 52% more aerosol holding capacity than the single layer uncharged nanofiber filter and 38% more capacity than the charged single-layer and the uncharged multilayer nanofiber filters. The multilayer PVDF electret filters have excellent filtration performance for long-term aerosol filtration and also great potential applications in the fields of personal health care and environmental protection.