To improve the catalytic effect of titanium dioxide under solar light, a silver film was deposited on the titanium surface by the vacuum evaporation method, and a femtosecond laser was used for the fabrication of the micro/nanostructured titanium dioxide and the incorporation of silver particles simultaneously. The results show that the photocatalytic efficiency of the Ag-TiO2 for removal of methylene blue is as high as 70% under simulated sunlight for 300min, which is 1.5 times of the photocatalytic efficiency of structured TiO2. This method based on direct processing of bulk materials can increase the specific surface area and solve the problems of traditional titanium dioxide’s recycling. Therefore, this technology shows high potential in the fabrication of environment-friendly titanium dioxide photocatalyst with high efficiency and large-scale and rapid production in factories.