Abstract: Disclosed are a Li+ doped metal halide scintillation crystal with a zero-dimensional perovskite structure, a preparation method and use thereof. The scintillation crystal has a chemical formula of Cs3-xCu2I5:xLi, where x is in a range of 0.003 to 0.3. The method for preparing the scintillation crystal comprises the steps of: weighting and fully mixing a CuI powder, a CsI powder and a LiI powder in a molar ratio of 2:(3-x):x in an inert atmosphere to obtain a mixed powder, and growing into the scintillation crystal from the mixed powder by Bridgman Stockbarger method. After excited, the scintillation crystal could emit a broadband blue light in a range of 350-550 nm, with an intensity much higher than that of the original pure component crystal. The existence of Li+ further expands the application of the scintillation crystals from X/?-ray detection to neutron detection.