We report the synthesis and characterization of CuO/Cu2O film supported on nanoporous alumina membranes (NAMs) and the photocatalytic properties in the removal of the organic pollutant methyl orange (MO). For this purpose, transparent nanostructured membranes were fabricated and sequentially modified with APTS ((3-aminopropyl)-trimethoxysilane) and EDTAD (ethylenediaminetetraacetic dianhydride) to form a highly functionalized surface with high density of carboxyl groups, which easily complex with copper cations. The Cu2+-modified membranes were annealed in a chemical vapor deposition (CVD) furnace to form a well-ordered nanostructured coating of CuO/Cu2O with photocatalytic properties. These modifications were followed by characterization with FT-IR and UV–visible spectra, X-ray photoelectron spectroscopy (XPS), field emission scanning electron microscopy (FE-SEM), and energy dispersive X-ray spectroscopy (EDS). Finally, the photocatalytic performance of the NAM-CuO/Cu2O nanostructured membranes was tested in the aqueous removal of MO dye as a model reaction system. Our results revealed 50% photocatalytic removal of MO under continuous light irradiation for 2 h. The procedure presented in this work provides an adequate approach for the fabrication of nanostructured devices with photocatalytic properties for the degradation of organic compounds