It was shown that this kind of TiO2materials has dual-functions of light-scattering and dye adsorption. The DSSC prepared by using the TiO2 spheres as top-scattering layer shows 7.2% power efficiency, and the EQE atthe wavelength of dye maximum adsorption is beyond 90%. There-fore, the TiO2 spherical materials prepared by electrospray and hydrothermal treatment are also important functional materials for DSSC applications.