Different kinds of membrane structures have been proposed for future space exploration and earth observation. However, due to the low stiffness, high flexibility, and low damping properties, membrane structures are likely to generate large-amplitude (compared to the thickness) vibrations, which may lead to the degradation of their working performance. In this work, the governing equations are established at first, taking into account the modal control force induced by the polyvinylidene fluoride (PVDF) actuator. The optimal vibration control of the membrane structure is explored subsequently. A square PVDF actuator is attached on the membrane to achieve the vibration suppression. The influence of actuator position and control gains on the vibration control performance are studied. The optimal criteria for actuator placement and energy allocation are developed. Several case studies are numerically simulated to demonstrate the validity of the proposed optimization criteria. The analytical results in this study can serve as guidelines for optimal vibration control of membrane structures. Additionally, the proposed optimization criteria can be applied to active control of different flexible structures.