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The metal ion-implantation of titanium oxide with various transition metal ions was carried out by applying by high voltage acceleration. The subsequent calcination of the implanted TiO2 in oxygen at around 723 K resulted in a large shift in the absorption spectra of the TiO2 toward visible light regions, its extent being dependent on the amount and the kind of metal ions implanted. Such metal ion-implanted titanium oxide catalysts were active in carrying out various photocatalytic reactions such as the decomposition of NO into N2, O2 and N2O at 275 K under irradiation with visible light longer than 450 nm. The application of this advanced, high energy metal ion-implantation method enables the novel design of titanium oxide photocatalysts which can absorb and initiate vital reactions under visible light and will contribute to the development of catalytic systems utilizing solar energy.