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Understanding the structural dynamics of lead-halide perovskites is essential for their advanced use as photovoltaics. Here, the structural dynamics of the CH3NH3 cation and PbBr6 octahedra in the perovskite CH3NH3PbBr3 were studied via nuclear magnetic resonance (NMR) to determine the mechanism of the transition from the tetragonal to cubic phase. The chemical shifts were obtained by 1H, 13C, and 207Pb magic angle spinning NMR and 14N static NMR. The chemical shifts of the 1H nuclei in CH3 and NH3 remained constant with increasing tem