A platinum subnanocluster catalyst composed of 12窶�toms was synthesized using a phenylazomethine dendrimer, which can assemble twelve PtCl4 units by stepwise complexation, followed by reduction to Pt(0) . Unreactive olefins that were not activated by conventional 2窶�m Pt nanoparticles were successfully hydrogenated by the subnanocluster. EWG=electron-withdrawing group.