We present a light-harvesting strategy that utilizes organic donor molecules to achieve sensitized metal-to-ligand charge transfer (MLCT) based emission. In this scheme, coumarin dye molecules are covalently linked to the periphery of diimine ligands in Ru(II) inorganic complexes that display MLCT excited states. Our findings suggest that the singlet-singlet energy transfer strategies traditionally employed in artificial light-harvesting arrays can be adapted to incorporate MLCT excited states.