To improve photocatalytic efficiency, graphene/Ag/TiO2 nanotube catalyst was synthesized, and its surface characteristics and photocatalytic activity investigated. For deposition of Ag nanoparticles on the TiO2 nanotubes, a polymer compound containing CH3COOAg/poly(Llactide) was utilized, and the silver particles were precipitated by reducing the silver ions during the annealing process. Graphene deposition on the Ag/TiO2 nanotubes was achieved using an electrophoretic deposition process. Based on the dye degradation results, it was determined that the photocatalytic efficiency was significantly affected by deposition of silver particles and graphene on the TiO2 catalyst. Highly efficient destruction of the dye was obtained with the new graphene/Ag/TiO2 nanotube photocatalyst. This may be attributed to a synergistic effect of the graphene and Ag nanoparticles on the TiO2 nanotubes.