TiO2/graphene nanocrystals are synthesized at 200 ℃ with graphene and Ti(OC4H9)4 as precursors by hydrothermal synthesis method, which is fabricated on fluorine-doped tin oxide (FTO) and TiO2 nanoarray films by screen-printing.The composite films are evaluated with scanning electron microscopy (SEM) and photovoltaic tests. The result shows that we print TiO2/graphene nanocrystals on the TiO2 nanoarrays to prepare the photoanode of dye-sensitized solar cells by the double-layer structure of “nanocrystal+nanoarray”, which increases the absorbability for dye and absorption of ultraviolet-visible. The efficiency of the cell which uses TiO2 nanoarray coated by TiO2/graphene nanocrystals film as photoanode increases by 35% comparing with the TiO2/graphene nanocrystals film, and the highest efficiency is 3.53%.