The atomic dynamic behaviors of formamidinium lead iodide [HC(NH 2 ) 2 PbI 3 ] 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(NH 2 ) 2 + , FA + ] of FAPbI 3 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 (C 2 ) rotation along the N•••N axis and a four-fold (C 4 ) rotation along the C−H axis in the tetragonal phase, and eventually to local disordered motion as a partial C 4 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.