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Highly photoactive, graphene-wrapped anatase TiO2 nanoparticles are synthesized through one-step hydrothermal reduction of graphene oxide (GO) and TiO2 crystallization from GO-wrapped amorphous TiO2 NPs. Graphene-TiO2 nanoparticles exhibit a red-shift of the band-edge and a significant reduction of the bandgap (2.80 eV). Graphene-TiO2 nanoparticles possess excellent photocatalytic properties under visible light for the degradation of methylene blue.