The incorporation of metal oxide nanoparticles (NPs) in fiber filters is an effective approach to enhance the specific surface area and surface roughness of the fiber, hence improving their efficiency for fine dust capture and other gas treatment or biological applications. Nevertheless, uneven distribution of NPs limits their practical applications. In this study, a commercial silane coupling agent (3-methacryloxypropyltrimethoxysilane) was used to improve the dispersion of zinc oxide (ZnO) NPs in thin polyacrylonitrile fibers. Scanning electron microscopy (SEM) revealed that the fibers incorporating the silane-modified NPs exhibited better distribution of NPs than those prepared with pristine ZnO NPs. The silane modification enhanced the specific surface area, surface roughness, and fiber porosity. In particular, the nanofiber filter incorporating 12 wt% ZnO NPs modified with 0.5 g silane per g of ZnO NPs maintained a filtration efficiency of 99.76% with a low pressure drop of 44 Pa, excellent antibacterial activity, and could decompose organic methylene blue dye with an efficiency of 85.11% under visible light.