Solar sail can merely make use of solar radiation pressure (SRP) force as the thrust for space missions. The attitude dynamics is obtained for the highly flexible solar sail with control vanes, sliding masses, and a gimbaled control boom. The vibration equations are derived considering the geometric nonlinearity of the sail structure subjected to the forces generated by the control vanes, solar radiation pressure (SRP), and sliding masses. Then the dynamic models for attitude/vibration controller design and dynamic simulation are obtained, respectively. The linear quadratic regulator (LQR) based and optimal proportional‐integral (PI) based controllers are designed for the coupled attitude/vibration models with constant disturbance torques caused by the center‐of‐mass (cm)/center‐of‐pressure (cp) offset, respectively. It can be concluded from the theoretical analysis and simulation results that the optimal PI based controller performs better than the LQR based controller from the view of eliminating the steady‐state errors. The responses with and without the geometrical nonlinearity are performed, and the differences are observed and analyzed. And some suggestions are also presented.