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This study evaluates the removal of several dyes with different charge properties, i.e., anionic (Acid Red 88), cationic (Basic Red 13), and neutral (Basic Red 5) using transition metal-doped TiO₂ supported on a high-surface-area activated carbon. Experimental results confirm the successful deposition of TiO₂ and the derivatives (Zr-, Cu-, and Ce-doped samples) on the surface of the activated carbon material and the development of extended heterojunctions with improved electronic properties. Incorporating a small percentage of dopants significantly improves the adsorption properties of the composites towards the three dyes evaluated, preferentially for sample AC/TiO₂_Zr. Similarly, the photodegradation efficiency highly depends on the nature of the composite evaluated and the characteristics of the dye. Sample AC/TiO₂_Zr demonstrates the best overall removal efficiency for Acid Red 88 and Basic Red 5—83% and 63%, respectively. This promising performance must simultaneously be attributed to a dual mechanism, i.e., adsorption and photodegradation. Notably, the AC/TiO₂_Ce outperformed the other catalysts in eliminating Basic Red 13 (74%/6 h). A possible Acid Red 88 degradation mechanism using AC/TiO₂_Zr was proposed. This study shows that the removal efficiency of AC/TiO₂ composites strongly depends on both the material and pollutant.