Periodicmesoporousorganosilicaderivatives (PMOs) that bear a highdensity of Ru and Ir complexes on pore walls were synthesized using a unique two‐step approach: 1) synthesis of PMO containing phenylpyridine bridging groups in the pore walls, and 2) post‐synthetic formation of metalcomplexes using the phenylpyridine groups as chelating ligands (see picture).