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Among chemical water pollutants, Cr(VI) is a highly toxic heavy metal; solar photocatalysis is a cost-effective method to reduce Cr(VI) to innocuous Cr(III). In this research work, an efficient and economically feasible ZnO/CuO nanocomposite was grafted onto the polyester fabric ZnO/CuO/PF through the SILAR method. Characterization by SEM, EDX, XRD, and DRS confirmed the successful grafting of highly crystalline, solar active nanoflakes of ZnO/CuO nanocomposite onto the polyester fabric. The grafting of the ZnO/CuO nanocomposite was confirmed by FTIR analysis of the ZnO/CuO/PF membrane. A solar photocatalytic reduction reaction of Cr(VI) was carried out by ZnO/CuO/PF under natural sunlight (solar flux 5–6 kW h/m2). The response surface methodology was employed to determine the interactive effect of three reaction variables: initial concentration of Cr(VI), pH, and solar irradiation time. According to UV/Vis spectrophotometry, 97% of chromium was removed from wastewater in acidic conditions after four hours of sunlight irradiation. ZnO/CuO/PF demonstrated reusability for 11 batches of wastewater under natural sunlight. Evaluation of Cr(VI) reduction was also executed by complexation of Cr(VI) and Cr(III) with 1, 5-diphenylcarbazide. The total percentage removal of Cr after solar photocatalysis was carried out by AAS of the wastewater sample. The ZnO/CuO/PF enhanced the reduction of Cr(VI) metal from wastewater remarkably. [ABSTRACT FROM AUTHOR]