AbstractHigh‐sensitivity wearable radiation detectors are essential for personnel protection in radiation environments such as defense, nuclear facilities, and medical fields. Traditional detectors using bulk crystals lack flexibility, and emerging perovskite films suffer from lead toxicity and poor charge transport. Herein, lead‐free photoferroelectric hybrid metal halide perovskite flexible membranes for wearable detectors are presented, offering superior X‐ray response with sensitivities up to 7872 ± 517 µC Gyair−1 cm−2 at 50 V bias and 394 ± 67 µC Gyair−1 cm−2 in a self‐driven mode, detection limit of lower than 77 nGyair s−1, and excellent imaging capabilities. This exceptional performance is attributed to the spontaneous polarization that promotes efficient charge transport. Additionally, they show remarkable radiation stability, long‐term air stability, mechanical fatigue resistance, and water stability. They also exhibit efficient energy response under the Compton effect and meet the angle response requirements of the International Electrotechnical Commission standard for direct‐reading personal dose equivalent meters, paving the way for their integration into flexible, wearable dosimeters. These advancements have the potential to drive the realization of the next generation of flexible wearable radiation detectors.
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