Magnetically suspended sensitive gyroscopes (MSSGs) provide an interesting alternative for achieving precious attitude angular measurement. To effectively reduce the measurement error caused by dynamic imbalance, this paper proposes a novel compensation method based on analysis and modeling of the error for a MSSG. Firstly, the angular velocity measurement principle of the MSSG is described. Then the analytical model of dynamic imbalance error has been established by solving the complex coefficient differential dynamic equations of the rotor. The generation mechanism and changing regularity of the dynamic imbalance error have been revealed. Next, a compensation method is designed to compensate the dynamic imbalance error and improve the measurement accuracy of the MSSG. The common issues caused by dynamic imbalance can be effectively resolved by the proposed method in gyroscopes with a levitating rotor. Comparative simulation results before and after compensation have verified the effectiveness and superiority of the proposed compensation method.