CuInS2quantum dots have been deposited onto mesoporous TiO2films on TCO glass substrate via successive ionic layer absorption and reaction process (SILAR) by using three different routes and post-deposition annealing in sulfur ambiance. The influence of the deposition sequence of the In-S and Cu-S on the microstructure of CuInS2sensitized TiO2electrodes and the photovoltaic performance of the solar cells have been investigated. The microstructure of CuInS2sensitized TiO2electrodes has been investigated by using X-ray diffraction (XRD), Raman spectra, scanning electron microscopy (SEM), and energy dispersive spectroscopy (EDS) analysis. The optical absorption property of the electrodes has been detected by using UV-Vis spectroscopy, and the photovoltaic performance of CuInS2quantum dots sensitized solar cells has been determined by cyclic voltammetry measurement. It has been found that when the Cu-S was deposited prior to In-S, the chalcopyrite phase CuInS2could not be observed due to the sublimation of InxS during the annealing under low pressure. A small amount of CuInS2has been detected when In-S and Cu-S was deposited alternately onto the TiO2films. However, chalcopyrite phase CuInS2can be obtained when In-S was deposited prior to Cu-S, and a relative high efficiency of ca. 0.92% (Voc= 0.35V, Jsc= 8.49 mA·cm-2, FF = 0.31) has been achieved via SILAR without KCN treatment and rapid thermal annealing.