We report on an experimental study aimed at optimizing the radiocatalytic properties of pure and copper-incorporated TiO 2 powders. This has been achieved by conducting crosschecked structural, optical and radiocatalytic studies. Structural and nanoscale analyses show evidence of internal doping by Cu 2+ in the TiO 2 lattice that leads to the reduction of the optical band gap down to 1.5 eV. The effect of gamma radiation on the radiocatalytic activity of these catalysts was studied by degradation of methylene blue as a model pollutant. It was found that the addition of Cu-doped TiO 2 (anatase) powders improves significantly the pollutant degradation, as compared to photocatalysis. The doping and the annealing temperature's impact on the structural, optical and radiocatalytic efficiencies are highlighted and correlated.