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In this study, a visible-light-driven P25 TiO2 was prepared upon surface modification with a colored organic hybrid of phosphotungstic acid that makes titanium dioxide suitable for photocatalytic degradation of organic pollutants under visible and sunlight irradiation. Visible shifting of the photocatalytic activity of surface-modified TiO2 was examined by studying the decolorization of methylene blue (MB) and rhodamine B (RhB). The results show that colored TiO2 is, unlike bare TiO2, a good photocatalyst in the degradation of dyes under visible and sunlight irradiation. Surface-modified Al2O3 and reduced graphene oxide (RGO) with organic hybrid of phosphotungstate failed to degrade RhB under sunlight irradiation, which prove the role of TiO2 in the photochemical process.