Immobilization of transition-metal catalysts on solid supports has practical benefits such as catalyst separation and reuse. However, in many cases, their catalytic activities were decreased compared to the homogeneous counterparts due to unfavorable interactions between the active site and the solid surface. To produce highly active heterogeneous transition-metal catalysts, we recently designed and synthesized multi-point solid-supported phosphines as supporting ligands. Owing to spatial isolation of the P centers on the solid supports, these immobilized phosphines allowed controlled metal coordination, which was effective to produce coordinatively unsaturated metal species. Thus, the multi-point solid-supported phosphines showed high ligand performance in various transition-metal catalysis, enabling challenging molecular transformations that were difficult with conventional homogeneous catalyst systems.