A series of Ru(II)L2L′ (L = 2,2′-bipyridyl, L′ = 2,2′-bipyridine-5,5′-dicarboxylic acid), RuDCBPY, -containing zirconium(IV) coordination polymer thin films have been prepared as sensitizing materials for solar cell applications. These metal–organic framework (MOF) sensitized solar cells, MOFSCs, each are shown to generate photocurrent in response to simulated 1 sun illumination. Emission lifetime measurements indicate the excited state quenching of RuDCBPY at the MOF–TiO2 interface is extremely efficient (>90%), presumably due to electron injection into TiO2. A mechanism is proposed in which RuDCBPY-centers photo-excited within the MOF-bulk undergo isotropic energy migration up to 25 nm from the point of origin. This work represents the first example in which a MOFSC is directly compared to the constituent dye adsorbed on TiO2 (DSC). Importantly, the MOFSCs outperformed their RuDCBPY–TiO2 DSC counterpart under the conditions used here and, thus, are solidified as promising solar cell platforms.