An extremely easy method is presented for producing surfactant-free films of nanocrystalline TiO2 at room temperature with excellent mechanical stability when deposited on glass or plastic electrodes for dye-sensitized solar energy conversion. Prolonged magnetic stirring of commercial TiO2 nanoparticles (Degussa P25) in either ethanol or water results in highly homogeneous dispersions which are used to prepare TiO2 films with surface properties which depend on the solvent used for dispersing the particles, even after sintering. The optical and mechanical properties of films cast from ethanol and water dispersions are compared, and differences in the extent of surface defects and dye binding are observed. Optical absorption, photoluminescence, and resonance Raman spectra of TiO2 films sensitized with Ru(4,4'-dicarboxylic acid-2,2'-bipyridine)(2)(NCS) 2 ("N3") reveal that the electronic coupling of the dye and semiconductor depends on the surface structure of the film which varies with film preparation. Current-voltage data for illuminated and dark dye-sensitized solar cells are obtained as a function of film preparation, and results are compared to spectroscopic data in order to interpret the microscopic basis for variations in solar cell performance, especially with regard to sintered versus unsintered TiO2 films. The results suggest that surface traps associated with oxygen vacancies play a critical role in determining the efficiency of dye-sensitized solar energy conversion through their influence on the binding and electronic coupling of the dye to the semiconductor.