This research explored the use of a partially cross-linked graft copolymer (PCLNPG) as an innovative nanopolymer pore-forming agent to enhance polyphenylsulfone (PPSU) membranes for protein separation applications. The study systematically examined the impact of incorporating PCLNPG at varying concentrations on the morphological and surface properties of PPSU membranes. A thorough characterization of the resulting PPSU-PCLNPG membranes was performed, focusing on changes in morphology, water affinity, porosity, pore size, and pore size distribution. The experimental findings demonstrated that the use of PCLNPG led to a significantly more porous structure, as confirmed by SEM analysis, with notable increases in porosity and pore size (nearly double). Additionally, the hydrophilicity of the PPSU membrane was remarkably enhanced. Performance evaluations revealed a substantial improvement in pure water flux, with the flux nearly tripling. The BSA retention was directly correlated with the concentration of the PCLNPG pore former for a loading range of 0.25–0.75 wt.%. The incorporation of PCLNPG also reduced the membrane fouling propensity by reducing both cake layer resistance (Rc) and pore plugging resistance (Rp). These results underscore the potential of PCLNPG-PPSU membranes for wastewater reclamation and nutrient recovery applications.