Abstract: Necessary to jointly address the two issues of easy TiO₂ electron-hole pairs recombination and low visible light response, spherical titanium dioxide(TiO_2（sp）) was first prepared from titanium oxide sulfate, and flake titanium dioxide(TiO_2（sh）) was prepared from tetrabutyl titanate. Then, by modifying ethylenediamine, N-doped titanium dioxide(N-TiO_2（sp） and N-TiO_2（sh）) was created. Then graphene oxide（GO） was prepared by the Hummers method, followed by ammonia modification to obtain nitrogen-doped graphene（NG）. Finally, N-TiO_2（sp） or N-TiO_2（sh） were loaded by the one-pot hydrothermal method to produce five samples of spherical N-doped TiO₂/N-doped graphene(N-TiO_2（sp）/NG) and five samples of sheet N-doped TiO₂/N-doped graphene(N-TiO_2（sh）/NG), separately. The structures were characterized by SEM, TEM, XRD, BET, XPS, FT-IR and UV-vis, and the synergistic photocatalytic activity of 2D NG loaded 0D/2D N-TiO₂ hybrids with different contents for X3B under visible light was investigated. The results show that: because nitrogen participates in the hybridization of the two, N-TiO₂ and NG have synergistic enhancement effect to improve photocatalytic activity, the light absorption range is extended to the visible region, the photogenerated electron-hole pairs recombination is inhibited, and the photocatalytic activity is improved. The 2D/2D contact N-TiO_2（sh）/NG3 hybrid material has the best synergistic catalytic effect, and the degradation rate of X3B by hybrid material reaches 98.5% in 50 min under simulated sunlight, which is 6.6 times that of TiO₂.