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A cylindrical resonator gyroscope is a kind of Coriolis gyroscope, which measures angular velocity or angle via processing of the standing wave. The symmetry of a cylindrical resonator is destroyed by different degrees of geometric nonuniformity and structural damage in the machining process. The uneven mass distribution caused by the asymmetry of the resonator can be expressed in the form of a Fourier series. The first three harmonics will reduce the anti-interference ability of the resonator to the external vibration, as well as increase the angular random walk and zero-bias drift of the gyroscope. In this paper, the frequency split of different modes caused by the first three harmonic errors and the displacement of the center of the cylindrical resonator bottom plate are obtained by simulation, and the relationship between them is explored. The experimental results on five fused silica cylindrical resonators are consistent with the simulation, confirming the linear relationship between the n = 1 frequency split and second harmonic error. A method for evaluating the first three harmonic errors of fused silica cylindrical resonators is provided.