Frequent outbreaks of emerging infectious diseases (EIDs) make personal protective filter media in high demand. Electrospun nanofibrous materials are proved to be very effective in resisting virus-containing fine particles owing to their small fiber diameters; however, hindered by the intrinsic close-packing character of fine fibers, electrospun filters suffer from a relatively high air resistance, thereby poor breathing comfort. Here, we report a biomimetic and one-step strategy to create ultrafine and curly wool-like nano-fibers, named nano-wool, which exhibit fluffy assembly architecture and powerful electret effect. By achieving the online self-crimp and in-situ charging of nanofibers, the curly electret nano-wool shows a small diameter of similar to 0.6 mu m (two orders of magnitude lower than natural wool: similar to 20 mu m) and an ultrahigh porosity of 98.7% simultaneously, together with an ultrahigh surface potential of 13260 V (one order of magnitude higher than previous filters). The structural advantages and powerful electret effect enable nano-wool to show excellent filtration efficacy (>99.995% for PM0.3) and low air resistance (55 Pa). Additionally, nano-wool can be easily scaled up, not only holding great industrial prospect in personal protective respirators, but also paving the way for developing next-generation wool in a cost-efficient and multifunctional form. (C) 2020 Elsevier Inc. All rights reserved.