Titanium dioxide (TiO2) is widely used, studied, and synthesized using different methodologies. By a modification of the material, it can be applied to wastewater treatment. A combined sputtering-laser ablation setup was used to deposit TiO2 thin films modified, individually and simultaneously, with gold (Au) and silver (Ag). To investigate the effect of the metal incorporation in titanium and its impact on the photocatalytic activity, with dye discoloration as a pollutant compound model, the deposited films were characterized by UV–Vis, photoluminescence, and Raman spectroscopies, as well as by parallel beam X-ray diffraction. The results showed that films with different Au and Ag loads, and an 18 nm average crystallite size, were obtained. These metals have an essential effect on the deposited film’s compositional, structural, and optical properties, directly reflected in its photocatalytic activity. The photocatalytic test results using UV-Vis showed that, after 1 h of applying a 4.8 V electric voltage, a discoloration of up to 80% of malachite green (MG) was achieved, using ultraviolet (UV) light.