Molecular modification of dye-sensitized, mesoporous TiO2 electrodes changes their electronic properties. We show that the open-circuit voltage (Voc) of dye-sensitized solar cells varies linearly with the dipole moment of coadsorbed phosphonic, benzoic, and dicarboxylic acid derivatives. A similar dependence is observed for the short-circuit current density (Isc). Photo voltage spectroscopy measurements show a shift of the signal onset as a function of dipole moment. We explain the dipole dependence of the Voc in terms of a TiO2 conduction band shift with respect to the redox potential of the electrolyte, which is partially followed by the energy level of the dye. The Isc shift is explained by a dipole-dependent driving force for the electron current and a dipole-dependent recombination current.