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Scintillators with high light yield, spatial resolution, and detection sensitivity are desirable for X‐ray imaging. Howerer, it remains challenging to improve the light yield and radiation detection capability of alkali metal rare‐earth fluoride (ALnF4). Herein, a type of Cu2+ ion heterovalent co‐doped LiLuF4:Tb,Cu microcrystalline scintillation material with high light yield, persistent, and thermostimulated luminescence is obtained by defect engineering. The heterovalent codoping strategy not only increases the radioluminescence (RL) intensity, but also introduces more carrier traps in the material to enhance the long‐afterglow and thermoluminescence intensity of LiLuF4:Tb microcrystals. After doping of 3 mol% Cu2+ ions, the RL efficiency is increased by 88.61%, and the X‐ray detection limit of LiLuF4:Tb,Cu reaches 2.7928 nGy·s‒1. This detectivity is considerably lower than the medical imaging requirements (5.5 µGy·s‒1). Furthermore, a large‐area flexible scintillation film of dimensions 30 × 30 cm2 is prepared to achieve high spatial resolution X‐ray imaging of 22 LP mm−1@MTF(modulation transfer function) = 0.2. Besides, this flexible film enables X‐ray imaging of curved objects and stores optical information for >48 h. This work provides a paradigm for improving the RL intensity and X‐ray detection sensitivity of alkali rare‐earth fluorides by crystal defect engineering, and enriches X‐ray high resolution extended imaging applications. [ABSTRACT FROM AUTHOR]

X‐ray flat‐panel detectors are widely used for nondestructive detection of internal information in medical radiography and industrial applications. However, a persisting challenge is the application of radiography on highly curved 3D objects to realize flexibility and information storage for the fabrication of flexible large‐area X‐ray detectors. This study demonstrates a halide‐based double perovskite Cs2Na0.9Ag0.1LuCl6:Dy3+ by a hydrothermal reaction. The as‐prepared crystals exhibit afterglow features through a co‐doping strategy of Dy3+ and Ag+ ions. The double perovskite material with doping modification exhibits excellent scintillation properties with high sensitivity, low detection limit, and high radiation stability. In addition, flexible scintillator detectors are fabricated with an area of 8.0 × 6.0 cm2 by the blade‐coating strategy, which has a high spatial resolution of 11.2 lp mm−1@MTF = 0.2. Based on the long afterglow properties, the Cs2Na0.9Ag0.1LuCl6:Dy3+ flexible film exhibits thermoluminescence after turning off the X‐ray, thereby having strong potential for X‐ray imaging of nonflat and irregular objects. [ABSTRACT FROM AUTHOR]