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With the improvement of the performance of optical equipment carried by on-orbit spacecraft, the requirements of vibration isolation are increasing. Passive isolation platforms are widely used, but the ability to suppress the low-frequency deterministic vibration disturbance is limited, especially near the system’s natural frequency. Therefore, an active vibration control strategy is proposed to improve passive isolation performance. In this paper, a Youla parameterized adaptive active vibration control system is introduced to improve the isolation performance of a piezo-actuated active–passive isolation structure. A linear quadratic Gaussian (LQG) central controller is first designed to shape the band-limited local loop of the closed-loop system. Then, the central controller is augmented into a Youla parameterized adaptive regulator with the recursive least square adaptive algorithm, and the Youla parameters (<i>Q</i> parameters) can be adjusted online to the desired value to suppress the unknown and time-varying multifrequency deterministic vibration disturbance. In the experiment, the residual vibration with respect to the combination of multiple frequencies is effectively suppressed by more than 20 dB on average, and a quick response time of less than 0.3 s is achieved when the deterministic residual vibration changes suddenly over time. The experimental results illustrate that the proposed adaptive active vibration control system can effectively suppress the low-frequency deterministic residual vibration.