This study aims to enhance the photocatalytic efficiency of CuxZn1-xAl2O4 (x = 0.0, 0.2, 0.4, 0.6, and 0.8) nanophotocatalysts synthesized via a sol-gel self-combustion method. Rietveld analysis confirmed the formation of single-phase spinels with a face-centered cubic structure and Fd-3m space group symmetry, while electron density distribution analysis supported the ionic character of bonding within the material. Subsequent UV-visible spectroscopy revealed that the addition of Cu(II) reduced the band gap from 4.66eV to 2.54eV, facilitating enhanced light absorption. Consequently, the catalyst with x = 0.8 deteriorated 95% of methyl orange (MO) and 93% of rhodamine-B (RhB) in 120minutes of visible light irradiation, following a pseudo-first-order kinetic model. The Cu0.8Zn0.2Al2O4 sample demonstrated significant reusability and stability, with degradation rates of 93-79% for RhB and 95-81% for MO after four cycles. Scavenging studies indicated that photoexcited holes (h), hydroxyl radicals (OH•), and superoxide radicals (O₂•⁻) were key factors in the degradation process. This study presents an improved approach for enhancing the photodegradation performance of the Cu0.8Zn0.2Al2O4 catalyst for pharmaceutical and wastewater treatment applications.