The resonance vibrations of LiTaO3 fast-shear overtone mode resonators with a ferroelectric inversion layer are analyzed. In addition to the fast-shear mode, the coupled extensional mode is considered. Different from most of the LiTaO3 resonators studied in the literature that are based on the slow-shear mode, the resonator in this paper operates with the fast-shear overtone mode. Results show that the capacitance ratio assumes maxima at two resonances, which are identified to be the second overtone modes of fast-shear and extension, respectively. It is found that the thickness of the inversion layer has obvious influences on the capacitance ratio of fast-shear and extensional modes. This condition may provide a simple method to adjust capacitance ratios of piezoelectric resonators. The influence mechanisms are also discussed. Besides, the effect of the cut angle of the crystal on the mode shape of vibrations is also investigated. The results can be used as important basis of parameters designs of LiTaO3 resonators operating on the fast-shear overtone mode.