Large flexible space structures (LFSS), such as solar panels and synthetic aperture radar antennae, are widely employed in spacecraft. Owing to their structural peculiarities in addition with the special environment in outer space, it is easy to be aroused for the structural vibration of LFSS. This kind of vibration is very harmful to spacecraft. In this paper, we proposed a new mechanism for the vibration control of LFSS. An embedded smart device with a piezoelectric ceramic stack was built up, also. First, the nonlinear theory of structural vibration coupled with inner forces was deduced. Second, the basic principle of the new mechanism with the piezoelectric ceramic stack was expounded. Third, the smart device manufacturing and the embedded techniques were introduced. Finally, taking several solar panel structures as illustrative examples, we carried out both digital simulations and ground experiments. The research results showed us that the proposed new mechanism is quite effective to the vibration control of LFSS. This paper gives a new way to solve the vibration control problem of LFSS, especially for those with low frequencies, which is very valuable for improving the accuracy and performance of spacecraft.