Enhancing the properties and structure of the ultrafiltration (UF) membrane via rational manipulation is important to optimize their perm-selectivity performance. To overcome the permeance-selectivity trade-off of nanocomposite membranes, Zirconium dioxide nanofibers (ZrO2 NFs) was synthesized in nano-micro size and then incorporated into the polysulfone (PSf) membrane. The effect of different concentrations of ZrO2 NFs on the membrane properties and performance were investigated. Compared to the pristine PSf membrane, the nanocomposite membranes exhibited a remarkable enhancement in the physiochemical properties, mechanical properties, and the overall performance. The results showed that the nanocomposite membrane (M3, 0.5% ZrO2 NFs) possesses the highest flexibility and tensile strength (43% higher than the pristine PSf). The enhancement of the wettability and enlarge the pore size (2.6 times increase) of this nanocomposite membrane, resulting in a remarkably heightened the pure water permeability (Jw1; 255.8 L m−2 h−1 bar−1). As a result, it achieved the highest permeability during the filtration of BSA solution with no decline in the BSA rejection. Furthermore, compared to the pristine PSf membrane, all nanocomposite membranes exhibited higher mechanical properties. This novel strategy of incorporating the nanofibers, instead of nanoparticles, offers significant opportunities to exploit the various inorganic nanofibers in the fabrication of diverse nanocomposite membrane types.