We have conducted a quantitative analysis of light-harvesting efficiency and electron-transfer yield for solar cells employing ruthenium dye, (tetrabutylammonium)2 cis-(2,2‘-bipyridyl-4-COOH, 4‘-COO-)2(NCS)2ruthenium(II), sensitized nanocrystalline TiO2 films with a series of light-scattering magnitudes. The light-harvesting efficiency increases with the addition of relatively large particles to a transparent film, especially for near-infrared wavelengths. Excess addition, however, lowers the light-harvesting efficiency over the whole visible wavelengths owing to enhanced light reflection at the conducting glass/TiO2 interface. Following a rigorous calculation using the results obtained from the light-harvesting efficiency and the short-circuit photocurrent measurements, we demonstrate for the first time that the electron-transfer yield markedly decreases with increasing optical thickness, that is, film light-scattering magnitude, by a maximum of ≈60%. The origins of the change in the electron-transfer yi...