The increasing demand for efficient wastewater treatment technologies, driven by global population growth and industrialisation, highlights the necessity for advanced, reliable solutions. This study investigated the efficacy of a slurry photocatalytic membrane reactor (PMR) for the advanced removal of organic pollutants, quantified via chemical oxygen demand (COD), under natural and simulated solar light irradiation. Employing two variants of iron-doped titania as photocatalysts and a polysulfone-based polymeric membrane for the separation process, the investigation showcased COD removal efficiencies ranging from 66−85% under simulated solar light to 52−81% under natural sunlight over a 7 h irradiation period. The overall PMR system demonstrated COD removal efficiencies of 84−95%. The results confirmed the enhanced photocatalytic activity afforded by iron doping and establish solar-powered slurry PMRs as an effective, low-energy, and environmentally friendly alternative for the advanced treatment of municipal wastewater, with the research providing valuable insights into sustainable water management practices.