Due to energy-efficient and green processes of photocatalysis, the visible-light-driven photocatalytic organic synthesis has developed greatly in the last decade. The well-known photocatalysts, Rull-polypyridyl complexes, have been extensively exploited in the synthesis of various chemicals. However, homogeneity of Ru-II-polypyridyl complexes makes their recycling difficult. Here, we show an effective strategy for boosting photocatalysis by incorporating [Ru-II(bpy)(3)] into a radical metal-organic framework (FJI-Y2). Recyclable photocatalyst FJI-Y2 can efficiently catalyze the cross-dehydrogenative coupling reactions of N-phenyltetrahydroisoquinoline derivatives with phosphite esters, forming medicinal a-aminoquinoline phosphonates. More importantly, the photocatalytic efficiency of FJI-Y2 is actually higher than its homogeneous counterpart [Ru-II(bpy)(3)]Cl-2, because multiple intermolecular interactions between 1,4,5,8-naphthalenediimide radicals and [Ru-II(bpy)(3) induce optimal photoinduced electron transfer process to expedite chemical conversion and recycling of catalysts. It is envisioned that MOFs containing radicals can be ideal platforms to incorporate more noble-metal photocatalysts for promoting photocatalysis.