Photocatalytic hydrogen production and uranium reduction can solve the problems of energy crisis and environmental pollution. Here, bismuth nanocluster loaded on N-doped porous carbon (Bi0/NC) with “memory catalysis” effect was prepared through a Bi-MOF precursor pyrolysis strategy for H2 generation and UO22+ reduction. The photocatalyst achieved an enhanced H2 production rate of 12.8 mmol g−1 h−1 and an improved UO22+ removal ratio of 95.9 %, which was 3.2 and 1.8 times as pristine carbon material, respectively. Moreover, both the H2 generation and UO22+ reduction showed a sustained activity under dark condition. Improved activity is ascribed to the optimized electronic property and the enhanced charge separation in Bi0/NC, which can be proved by the DFT calculation of projected density of state, Fermi level and charge density difference. This work provides a new strategy to realize the continuous H2 generation and U(VI) reduction in day and night.