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 (Q 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.