Magnetic liquid double suspension bearing (MLDSB) is composed of an electromagnetic system and hydrostatic system and its bearing capacity and stiffness can be greatly improved. It is very suitable for occasions of medium speed, heavy load, and starting frequently. Due to the gyroscopic effect and interference between the supporting system, the space state of the rotor can be affected and the operation stability of the MLDSB can be reduced greatly. Therefore, the coupling features of the multi-degree of freedom (multi-DOF) system are analyzed and a decoupling controller is designed and verified in the paper. Firstly, the paper introduces the structural characteristics, stress forms, and control regulation mechanism. Then, the mathematical transfer function of the multi-DOF supporting system is established and the coupling principle is revealed. The state feedback decoupling controller is designed by means of a state feedback decoupling, and its decoupling effect is analyzed by the Simulink module. Finally, the single-DOF decoupling system is independently controlled by the use of the root locus method. The coupling characteristics between channel x and channel y are tested experimentally, and the decoupling controller is added and its effect tested. The results show that the state feedback decoupling controller can effectively reduce the coupling degree in the multi-DOF system and convert the multi-DOF coupling problem into a single-DOF independent control problem. The coupling effect of channel x and channel y is reduced by using the decoupling controller, with the subsequent displacement characteristic of the rotor increased, and then the operation stability of the MLDSB is improved greatly. This paper can enrich the support system of the MLDSB and provide a theoretical reference for stability control.