photo voltaics, perovskite solar cells have already exceeded 23% in power conversion efficiency in a short development period. [1][2][3][4] OMHPs have also become popular in many other optoelectronic applications, such as light-emitting diodes, [5,6] photodetectors, [7,8] and lasing applications. [9] Properties such as tunable band gaps, [10,11] low trap state densities, [12] and long carrier diffusion lengths make OMHPs a desirable material for a wide range of optoelectronic applications, as well as being a focus for other semiconducting device applications. [13,14] These fascinating optoelectronic properties have recently sparked a new interest for applications of OMHPs for high-energy radiation detectors, which are considered as a critical technology in many fields, including nuclear safeguards, nuclear forensics, and astrophysics. Notably, current solid-state detector technologies using classical semiconductors have many challenges that must be overcome for wide spread development. For example, Cadmium Zinc Telluride (CZT) is a commercial γ-ray detection semiconductor achieving reasonable resolution (≈2% at 662 keV) at room temperature. However, the complicated and costly high-quality crystal growth for this semiconductor fabrication prohibits its broad adaptation. Another example of a more cost-effective semiconductor is high purity Germanium, (HPGe) which achieves an impressive resolution, (≈0.2% at 662 keV) albeit under operation at liquid nitrogen temperatures. [15] Thus, achieving cost efficient, robust high resolution detection at ambient conditions has been a long-time aim for semiconductor γ-ray detectors. In this arena, lead-halide based perovskites have been proposed as a new generation semiconductors in γ -spectroscopy for its low-cost solution process and simple crystal growth for room temperature detectors. [16][17][18] The incorporation of high-Z elements (i.e., Pb) underscores the opportunity for enhanced photoelectric interaction probability. Large band gaps and high resistivities are also essential for highly sensitive operation in the resistive mode. [19] Moreover, the long carrier lifetime and decent ambipolar mobility give great potential for single photon counting and pulse mode radiation sensing. [15] Previous reports have shown promising proof-of-principle results for the application of perovskites as ionizing radiation In recent years, hybrid perovskite single crystalline solid-state detectors have shown promise in γ-ray spectroscopy. Here, the γ-ray photon induced electrical pulses are investigated, which are produced by perovskite solid-state detectors made with the commonly used methylammonium lead tribromide crystals with chlorine incorporation. Under low electric field detector operation, slow pulses generated by γ-rays with average rise times of 65 µs are observed, which decreases to 20 µs when a higher electrical field of 500 V cm −1 is applied. However, the baseline becomes noisy quickly, which prevents collection of clean pulses for spectra construction. Further, by systematic...