Due to low water fluxes, commercial ultrafiltration (UF) membranes used in water treatment need to be improved. High-quality UF membranes were fabricated from polysulfone (PSF)/titanium dioxide (TiO2) nanocomposite fibers as substrates using the spray pyrolysis method. The influence of nano-TiO2 on the UF nanocomposite membrane was studied. Scanning electron microscopy (SEM), contact angle, and porosity were evaluated to characterize the mechanical characteristics of the membranes. The results show that adding TiO2 to the substrates increased the hydrophilicity and porosity of the substrates. The pure water flux of the Thin Film Nanocomposite (TFN) membrane manufactured utilizing a PSF substrate coated with 0.1 wt% TiO2 nanoparticles (denoted as Pc 0.1) improved at a rate of 35.28 l/m2.h, and for a PSF substrate coated with 0.2 wt% TiO2 nanoparticles (denoted as Pc 0.2) improved at a rate of 44 l/m2.h. Additionally, increasing TiO2 nanoparticle loading to 0.1 and 0.2 wt. percent resulted in higher water flow over 20 l/m2.h PSF commercial membrane. The results of the UF performance show that Pc 0.2 membrane offered the most promising results, with a high-water flux than commercial membranes without nano-TiO2 (Pc).