The invention provides a CuI crystal growth method, which belongs to the field of crystal growth in photoelectric functional material technology. The method uses a low-temperature aqueous solution cooling method to grow crystals, using NH4Cl, NH4Br, NH4I, etc. as cosolvents, copper sheets as reducing agents, paraffin oil seals, growth temperature range of 30-60°C, and cooling rate of 0.1-0.5°C / day. The cooling method crystal growth technology adopted in the present invention has the advantages of low growth temperature, low solution viscosity, simple and easy device, and the growth process can be directly observed. The grown CuI crystal has high purity, good uniformity, and large size. The ultrafast scintillation crystal is expected to play an important role in the future measurement of ultra-high count rate electrons, γ-rays and X-rays. It is also used as a semiconductor material for solar cell materials, superconducting materials and photocatalytic materials.