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Two X-ray scintillators based on organic–inorganic hybrids were constructed by judiciously incorporating lanthanide cations and organic ligands within a single material. The obtained Eu-pbaand Tb-pbanot only feature excellent radiation, hydrolytic, and thermal stabilities but also exhibit a linear response to the X-ray dose rate with detection limits of 4.92 and 3.17 μGy s–1, respectively. We further present a flexible scintillator film fabricated by embedding Tb-pbain a polydimethylsiloxane (PDMS) polymer. Their incorporation enables X-ray imaging with a spatial resolution of approximately 10 lp mm–1. These results emphasize the potential of lanthanide organic–inorganic hybrids to achieve outstanding performance in X-ray scintillation and imaging.