The conversion of uranium(U) from soluble U(VI) into insoluble U(IV) by photocatalytic reduction is an implementable removal technology. In this investigation, two common MOFs photocatalysts (MOF-In, MOF-Ti) and the assembled MOF@COF (2D Schiff base, NH2-MIL-125(Ti)@TpPa-1) were applied for photocatalytic reduction of U(VI). These as-synthesized photocatalysts were characterized by XRD,SEM, TEM, XPS, DRS, EIS, photocurrent and Mott-Schottky plots. The results shown that the constructed NH2-MIL-125(Ti)@TpPa-1 heterojunction not only broadened the scope of visible light response to orange light (600 nm), but also expedited the separation of photogenerated carriers and facilitatedthe U(VI)photoreduction. Specially, the photoreduction removal rates of U(VI) were NH2-MIL-68(In) (55.6%), NH2-MIL-125(Ti) (57.7%), NH2-MIL-125(Ti)@TpPa-1 (81.6%), and the heterojunction of NH2-MIL-125(Ti)@TpPa-1 was about 1.5-fold higher than that of NH2-MIL-125(Ti). Meanwhile, during the photoreduction process, photogenerated electrons and superoxide radicalsplayed the dominant roles in converting U(VI) into U(IV). Moreover, the presence of active Ti3+and oxygen vacancycould effectively promotesuperoxide radicalgeneration and inhibit recombination of photogenerated carriers. Combined with the U(VI) adsorption by NH2-MIL-125(Ti)@TpPa-1 in previously studied, altogether, MOF@COF hybridization can play a synergistic role of adsorption-photocatalytic reduction in the practical application of U(VI) elimination. Therefore, it can be predicted that 2D COF-based hybridization materials have a brilliant application prospect in pollutant purification by solar energy.