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In article number 2001882, Pavao Andričević, László Forró, and co‐workers introduce the ‘oriented crystal‒crystal intergrowth’ method, yielding solution‐grown MAPbBr(3) crystals with volume and mass of over 1000 cm(3) and 3 kg. Its increased size, equipped with carbon electrodes, is utilized for sensitive gamma ray detection of a (60)Co source at the dose rate up to 2.3 Gy h(−1) at ambient conditions. [Image: see text]

Gamma‐rays (γ‐rays), wherever present, e.g., in medicine, nuclear environment, or homeland security, due to their strong impact on biological matter, should be closely monitored. There is a need for simple, sensitive γ‐ray detectors at affordable prices. Here, it is shown that γ‐ray detectors based on crystals of methylammonium lead tribromide (MAPbBr3) ideally meet these requirements. Specifically, the γ‐rays incident on a MAPbBr3 crystal generates photocarriers with a high mobility‐lifetime product, allowing radiation detection by photocurrent measurements at room temperatures. Moreover, the MAPbBr3 crystal‐based detectors, equipped with improved carbon electrodes, can operate at low bias (≈1.0 V), hence being suitable for applications in energy‐sparse environments, including space. The γ‐ray detectors reported herein are exposed to radiation from a 60Co source at dose rates up to 2.3 Gy h−1 under ambient conditions for over 100 h, without any sign of degradation. The excellent radiation tolerance stems from the intrinsic structural plasticity of the organic–inorganic halide perovskites, which can be attributed to a defect‐healing process by fast ion migration at the nanoscale level. The sensitivity of the γ‐ray detection upon volume is tested for MAPbBr3 crystals reaching up to 1000 cm3 (3.3 kg in weight) grown by a unique crystal growth technique., The largest halide perovskite crystal specimens are produced up to 3.3 kg. The increased size allows fabrication of sensitive γ‐ray detectors able to work under high dose rates (2.3 Gy h−1) for over 100 h, without any sign of degradation. The excellent radiation tolerance can be attributed to a defect‐healing process by fast ion migration at the nanoscale level.