We report here the utilization of atomic layer deposition to passivate surface trap states in mesoporous TiO 2 nanoparticles for solid-state dye-sensitized solar cells based on 2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenylamine)-9,9′-spirobifluorene (spiro-OMeTAD). By depositing ZrO 2 films with angstrom-level precision, coating the mesoporous TiO 2 produces over a two-fold enhancement in short-circuit current density, as compared to a control device. Impedance spectroscopy measurements provide evidence that the ZrO 2 coating reduces recombination losses at the TiO 2 /spiro-OMeTAD interface and passivates localized surface states. Lowfrequency negative capacitances, frequently observed in nanocomposite solar cells, have been associated with the surface-state mediated charge transfer from TiO 2 to the spiro-OMeTAD.