Worldwide environmental challenges pose critical problems with the growth of the global economy. Addressing these issues requires the development of an eco-friendly and sustainable catalyst for degrading organic dye pollutants. In this study, copper-doped magnesium aluminates (CuxMg1−xAl2O4) with x = 0.0–0.8 were synthesized using a citrate-based combustion route. The inclusion of Cu(II) significantly impacted the structural, microstructural, optical, and photocatalytic activity of the catalyst. Rietveld analysis of X-ray diffraction powder profiles revealed single-phase spinels crystallized in the face-centered cubic unit cell with \(\mathrm{Fd}\overline{3}\mathrm{m }\) space group. Chemical states of the ions, surface morphology, and elemental investigation were analyzed by X-ray photoelectron spectroscopy, field-emission scanning electron microscopy, and energy-dispersive X-ray spectroscopy, respectively. UV–visible and diffuse reflectance spectroscopies confirmed the reduction of the band gap due to Cu(II) doping, validated by first-principle investigations using the WIEN2k code. The catalyst with x = 0.8 showed higher photocatalytic efficacy (90% and 93%) for removing two azo organic dye pollutants, rhodamine B and methyl orange, respectively, within 120 min. Degradation kinetics followed a pseudo-first-order mechanism. The doped (0.8) sample was structurally and morphologically stable and reusable under visible irradiation, retaining performance after three runs. Scavenger studies confirmed hydroxyl and superoxide radicals’ involvement in the degradation. This work presents an effective approach to enhancing CuxMg1−xAl2O4 catalysts’ photodegradation performance, with potential applications in pharmaceuticals and wastewater remediation.
