Photocatalytic efficiency is closely correlated to visible-light absorption ability, electron transfer efficiency and catalytic center activity of photocatalysts, nevertheless, the concurrent management of these factors to improve photocatalytic efficiency remains underexplored. Herein, we proposed a sensitizer/catalyst dual regulation strategy on the polyoxometalate@Metal-Organic Framework (POM@MOF) molecular platform to construct highly efficient photocatalysts. Impressively, Ni-Sb