Organic-inorganic hybrid halide perovskites, represented by CH 3 NH 3 PbX 3 (X ¼ Cl, Br, I), have demonstrated excellent optoelectronic and radiation detection properties. [1-3] All-inorganic CsPbX 3 perovskites (X ¼ Cl, Br, I) with better long-term stability are also considered as promising materials for optoelectronic devices and semiconductor γ-ray detectors. [4-6] Recently, there has been a surge of interest in low-dimensional perovskites due to their high photoluminescence quantum yield (PLQY). For example, the crystal structure of Cs 4 PbBr 6 that consist of spatially isolated [PbBr 6 ] 4À octahedra surrounding with Cs þ ions can be regarded as a 0D structure at molecular level, which leads to an intense quantum confinement effect. Excitons are strongly confined at each [PbBr 6 ] 4À octahedron, enabling a high exciton binding energy of 353 meV and a high PLQY of between 42% and 45%. [7,8] Quite a few low-dimensional allinorganic perovskites with remarkable luminescent properties were also reported as sensitive and efficient scintillators. Bulk crystals of 0D Cs 4 CaI 6 :Eu, Cs 4 SrI 6 :Eu, and Cs 4 EuBr 6 perovskites, isostructural to K 4 CdCl 6 trigonal system, have excellent light yields from 51 800 to 78 000 photons MeV À1 and energy resolutions from 3.3% to 4.3% at 662 keV. [9,10] However, due to a small Stokes shift of Eu 2þ ions, these materials suffer from strong self-absorption effect when scaling-up crystal size. Nanocrystals of 0D CsPbBr 3 /Cs 4 PbBr 6 perovskites show a high light yield of 64 000 photons MeV À1 and a fast decay time of <10 ns. [11] Onedimensional materials were also reported as sensitive X-ray scintillators, such as Rb 2 CuBr 3 and Rb 2 CuCl 3. [12,13] In particular, the Rb 2 CuBr 3 , that is self-absorption free and nonhygroscopic, was reported to achieve an ultrahigh scintillation yield of 90 000 photons MeV À1. [12] All-inorganic 0D perovskite Cs 3 Cu 2 I 5 was recently reported as a highly efficient blue-emitting material with a PLQY of 91.2%, and regarded as promising for application in photodetectors, light-emitting diodes, and memristors afterward. [14-17] In 2020, Cs 3 Cu 2 I 5 nanocrystals were developed for X-ray imaging with a light yield of 80 000 photons MeV À1. [18] To the best of our knowledge, the X-ray and γ-ray detection capability of bulk Cs 3 Cu 2 I 5 single crystal has not been reported. Thus, the aim of this work is to study the physical and optical properties and the scintillation performance under X-ray and γ-ray radiation of high-quality Cs 3 Cu 2 I 5 perovskite single crystal grown by the Bridgman method. The 7 mm diameter single crystal of Cs 3 Cu 2 I 5 was grown by the vertical Bridgman method. High-purity powders of CsI (99.99%, Grirem Advanced Materials) and CuI (99.999%, Sigma-Aldrich) were used as raw materials. These starting materials were mixed consistent with stoichiometric ratio and loaded into a quartz ampoule in a glovebox with <0.1 ppm moisture and oxygen. The loaded ampoule was sealed under a vacuum of 10 À6 torr after drying at 180 C for ...