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As engineers strive to develop high-performance filtration membranes with structural alternatives, the challenges and costs of processing often limit creative innovation. Here, we describe a powerful yet economic strategy for fabricating multilevel structured nanofibrous membranes within a single filter medium, which is constructed by the accumulation of bimodal sized and silica nanoparticles (SiO₂ NPs) incorporated electrospun polyacrylonitrile (PAN) nanofibrous membranes. By simply varying the composition of precursor solutions and layer-by-layer assisted stacking structure, individual fibers within the medium can conformally be endowed with non-circular cross section, or rough surface to form a skeletal frame-worked membrane with complimentary filtration efficiency (99.989%) and pressure drop (117 Pa) for 300–500 nm NaCl aerosol particles. The results suggested that this cost-effective filter media could be …