To achieve the high-precision angular velocity and angular acceleration estimation of spacecraft under high dynamic conditions, a novel method based on single-gimbal magnetically suspended control moment gyroscope (SGMSCMG) configuration is proposed in this paper. Both the angular rates and angular accelerations have been resolved analytically, and their comparative estimation precision between the proposed method and the traditional one has been further analyzed in the presence of gyro error and installation error. Compared to the traditional three-orthogonal configuration method, the proposed one employs any three SGMSCMGs in the control actuator configuration instead of additional rate gyros. All the inertial coupling items are retained tactfully in the angular rate and angular acceleration solution by the proposed method. Thus, the relative estimation accuracy of the attitude rate depends only on the gyro error and its installation error in practice, which do not decay under high dynamic conditions anymore. And its corresponding angular acceleration estimation precision is determined by the size of angular velocity instead of angular acceleration under the given error condition. The semiphysical simulation results demonstrate the correctness and superiority of the proposed estimation method.