The atomic dynamic behaviors of formamidinium lead iodide [HC(NH2)2PbI3] are critical for understanding and improving photovoltaic performances. However, they remain unclear. Here, we investigate the structural phase transitions and the reorientation dynamics of the formamidinium cation [HC(NH2)2+, FA+] of FAPbI3 using neutron scattering techniques. Two structural phase transitions occur with decreasing temperature, from cubic to tetragonal phase at 285 K and then to another tetragonal at 140 K, accompanied by gradually frozen reorientation of FA cations. The nearly isotropic reorientation in the cubic phase is suppressed to reorientation motions involving a two-fold (C2) rotation along the N···N axis and a four-fold (C4) rotation along the C-H axis in the tetragonal phase, and eventually to local disordered motion as a partial C4 along the C-H axis in another tetragonal phase, thereby indicating an intimate interplay between lattice and orientation degrees of freedom in the hybrid perovskite materials. The present complete atomic structure and dynamics provide a solid standing point to understand and then improve photovoltaic properties of organic-inorganic hybrid perovskites in the future.