As a novel active semiconducting material for optoelectronics, organic‐inorganic hybrid perovskites have attracted much attention due to the special advantages of the high light absorption coefficient, long diffusion length and high charge carrier mobility. The single crystals with low defects and free grain boundaries can provide an ideal platform to study the intrinsic photophysical properties and show better performance compared with its amorphous or polycrystalline states. The excellent physical properties of perovskite single crystals make them applied in many fields of solar cells, photodetectors, light‐emitting diodes, lasers, catalysis, etc. Here, the recent progress in the single crystal growth, molecular structures and the bandgap engineering of organic‐inorganic hybrid perovskite single crystals are introduced. The perspective and the future challenge are also provided.