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Perovskite X-ray detectors are actively investigated because of their exceptional properties, including their significant attenuation coefficient, low defect density, excellent transport characteristics, easy growth, and high sensitivity to X-ray photons. However, perovskite-based high-energy X-ray detectors on the MeV scale are rarely explored. In this study, we investigate the optoelectronic characteristics and radiation detection capabilities of triple-cation Cs 0.05 FA 0.9 MA 0.05 PbI 3 single crystals (CSC) grown using the inverse temperature crystallization method. The CSCs with a reduced Goldschmidt tolerance factor owing to the presence of Cs and MA ions exhibit exceptional properties, including a bandgap of 1.447 eV, low dark current, and self-powered response to X-ray irradiation. The X-ray absorption rate of 36 keV exceeded 99% with a CSC thickness of 2 mm, demonstrating its strong stopping power. Moreover, the CSC detectors exhibit precise linear responses to varying X-ray doses and dose rates with R2 values close to 1 and relative standard deviation (RSD) values below 3% under all the tested conditions. In addition, the detector effectively detected high-energy X-rays of up to 15 MV with minimal variations in the RSD values. These findings highlight the potential of CSC as promising materials for high-performance X-ray detectors. • Triple-cation lead–halide perovskites for high-energy X-ray detection were studied. • CSC detector has uniform linear response to varying X-ray doses and rates. • CSC detector can detect high-energy X-rays of up to 15 MeV. • CSC demonstrated remarkable promise as excellent self-powered X-ray detectors. [ABSTRACT FROM AUTHOR]