This study investigates the effectiveness of electrospun nanofibrous filters in capturing polydisperse virus-containing aerosols and the subsequent release of viruses, in comparison with standard commercial filters used in respirators, military gas masks, and devices for airborne virus sampling. We assessed the performance of these filters in capturing and releasing polydisperse aerosols containing MS2 bacteriophage, as well as in their ability to filter monodisperse dioctyl phthalate aerosols measuring 0.185 μm and 0.3 μm in diameter. Our findings indicate that nanofibrous filters provide superior filtration efficiency for monodisperse aerosols, achieving a reduction in the concentration of penetrating aerosols by 2-3 orders of magnitude compared to their commercial counterparts. However, this enhanced efficiency is accompanied by a higher pressure drop and a lower quality factor, underscoring the need for further improvements. Additionally, our research confirms the feasibility of producing aligned nanofibers via multiple-jet needleless electrospinning, though alignment did not significantly impact filtration efficiency. Nanofibrous filters demonstrated filtration efficiency for aerosolized virus-containing particles that was comparable to or better than that of commercial filters. Notably, certain nanofibrous filters exhibited exceptionally low rates of viral aerosol capture and release, indicating a potential for virus neutralization. Moreover, filters made from water-soluble electrospun polyvinylpyrrolidone significantly outperformed those made from gelatin in terms of viral particle release, underscoring the potential of water-soluble electrospun materials in improving viral particle collection. Overall, our study highlights the significant promise of electrospun nanofibers in public health, especially in enhancing defenses against the transmission of viral aerosols.