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Copper metal halides have emerged as a strong contender in the scintillator field due to the self‐trapped excitons (STEs) mechanism. However, their development has been hindered by the preparation process. Single crystals have long growth cycles and cannot achieve large areas and flexibility. Quantum dots have a low yield and can easily cause chemical pollution, and the thickness of films prepared by the spin coating cannot be controlled. To address these challenges, a new method for preparing Cs3Cu2Cl5 using sequential vacuum evaporation is developed. This allows successful preparation of large‐area (≈100 cm2) and flexible films. The STEs mechanism of Cs3Cu2Cl5 gives it unique properties such as a large Stokes shift that reduces self‐absorption effects, and a wide full width at half‐maximum that improves coupling with photodiodes. Therefore, Cs3Cu2Cl5 is applied to X‐ray imaging with a light yield of ≈30 000 photons MeV−1, a spatial resolution of over 10 lp mm−1, and a low detection limit below 0.8 µGyair s−1. In addition, the flexible Cs3Cu2Cl5 film enables effective dynamic imaging and clear imaging on non‐planar objects. It also exhibits good resistance to harsh environments, maintaining good imaging performance after 150 days. It is believed that sequential vacuum evaporation provides an important idea for preparing scintillators. [ABSTRACT FROM AUTHOR]

Herein, the first study on the scintillation properties of CsCu2X3 and Cs3Cu2X5 (where X: Cl−, Br−, I−) is presented, describing their charged particle‐induced luminescence involving electrons, protons, α‐particles, and heavy ions, as well as revealing their capabilities on the timing and spectroscopic evaluation of single‐particle events. The thin layers are prepared with a simple and cost‐effective deposition procedure, without the incorporation of external dopants, exploiting the intrinsic radiative recombination observed in low‐dimensional perovskites. The combined effect of the high binding energy and localized stability of self‐trapped excitons, large Stokes shift, defect tolerance, and the high excitation density along the particle track leads to the emergence of boosted scintillation pulses. The observations demonstrate the first use of inorganic thin‐film scintillators with optical pulse characteristics and light yield competitive with doped single crystal scintillators, while also providing improved structural and functional stability under extreme environmental conditions. [ABSTRACT FROM AUTHOR]