In this paper, a novel tensioning and relaxing wearable system is introduced to improve the wearing comfort and load-bearing capabilities of knee exoskeletons. The research prototype of the novel system, which features a distinctive overrunning clutch drive, is presented. Through co-simulation with ANSYS, MATLAB, and SOLIDWORKS software, a comprehensive multi-objective optimization is performed to enhance the dynamics performance of the prototype. Firstly, the wearing contact stiffness of the prototype and the mechanical parameters of the relevant materials are simulated and fitted based on the principle of functional equivalence. And then, its equivalent nonlinear circumferential stiffness model is obtained. Secondly, to enhance the wearing comfort of the exoskeleton, a novel comprehensive performance evaluation index, termed wearing comfort, is introduced. The index considers multiple factors such as the duration of vibration transition, the acceleration encountered during wear, and the average pressure applied. Finally, through the utilization of this indicator, the system’s dynamics performance is optimized via multi-platform co-simulation, and the simulation results validate the effectiveness of the research method and the proposed wearable comfort index. The theoretical basis for the subsequent research on the effectiveness of prototype weight-bearing is provided.