In this study, we developed TiO2-coated aluminum (TiO2/Al) surfaces using eco-friendly methods to create efficient and environmentally friendly photoactive materials with the potential to enhance water purification systems. TiO2 particles were deposited onto aluminum foil surfaces via a spray method, followed by heat treatment at 200 °C for 15 min. The morphology of the TiO2/Al surfaces, both before and after photocatalytic treatment, was characterized using scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDS). The photocatalytic properties of these modified surfaces were evaluated through the degradation of rhodamine B (RB), methylene blue (MB), and methyl orange (MO) under simulated solar and UV–LED irradiation. Among the dyes tested, MO exhibited the highest degradation, influenced by factors such as absorption maximum, molecular structure, charge, and the number of condensed rings. The computational study of interactions between dye molecules and the combined nanoparticle revealed that the binding was the strongest in the case of MO dye. This study also explored the influence of varying the number of TiO2/Al surfaces in solution (one, five, and ten) on the photodegradation efficiency. The solution with five TiO2/Al surfaces demonstrated optimal performance, achieving a 16% degradation of RB. The reusability of the TiO2/Al surfaces was confirmed through five successive runs of RB degradation. The results indicate that TiO2/Al surfaces are a promising solution for addressing water contamination challenges and advancing sustainable water treatment practices.