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Metal halide crystals are bright but hygroscopic scintillator materials that are widely used in X‐ray imaging and detectors. Precipitating them in situ in glass to form glass ceramics (GCs) scintillator offers an efficient avenue for large‐scale preparation, high spatial resolution, and excellent stability. However, precipitating a high fraction of metal halide nanocrystals in glass to maintain high light yield remains a challenge. Herein, an ionic‐covalent hybrid network strategy for constructing GCs scintillator with high crystallinity (up to ≈37%) of BaCl2: Eu2+ nanocrystals is presented. Experimental data and simulations of glass structure reveal that the Ba2+‐Cl− clustering promotes the high crystallization of BaCl2 nanocrystals. The ultralow phonon energy (≈200 cm−1) of BaCl2 nanocrystals and good Eu reduction effect enable high photoluminescence inter quantum efficiency (≈80.41%) in GC. GCs with varied crystallinity of BaCl2: Eu2+ nanocrystals demonstrate efficient radioluminescence and tunable scintillator performance. They either outperform Bi4Ge3O14 single crystal by over 132% steady‐state light yield or provide impressive X‐ray imaging resolutions of 20 lp mm−1. These findings provide a new design strategy for developing bright transparent GCs scintillators with a high fraction of metal halide nanocrystals for X‐ray high‐resolution imaging applications. [ABSTRACT FROM AUTHOR]

[Display omitted] • MAPbBr 3 NCs are in-situ space-confined encapsulated in metal–organic frameworks. • bMOF⊃MAPbBr 3 realizes room-temperature scintillation and exceptional X-ray imaging. • bMOF⊃MAPbBr 3 shows enhanced stability against various stimuli and X-rays. • The role of the MOF and the mechanism of improved performance are elucidated. The development of perovskite nanocrystals (NCs) based composites with enhanced stability and exceptional photoelectric properties is of great significance for their application in scintillators for X-ray imaging, but it remains challenging. Herein, we demonstrate a novel and stable scintillator, achieved through a host–guest strategy involving the confinement of perovskite NCs, e.g., MAPbBr 3 NCs, in metal–organic frameworks (MOFs). The host MOF, bio-MOF-100 (denoted as bMOF), facilitates the in-situ space-confined formation of MAPbBr 3 NCs while providing quantum confinement, surface passivation, and protection to these guests. This host–guest strategy results in high exciton binding energy, bright and efficient luminescence, and significantly enhancing their stability against various factors such as air, heat, UV, solvents and X-ray irradiation. Consequently, this advancement prompts the transition of their application scenarios from the colloidal state to the solid state. The bMOF⊃MAPbBr 3 scintillator exhibits a linear response to X-ray with a detection limit determined to be 170 nGy air s−1. Moreover, the bMOF⊃MAPbBr 3 –PMMA scintillator screen demonstrates high-quality X-ray imaging with an impressive spatial resolution of 14.7 lp mm−1. This work provides a new avenue for the development of perovskite NCs-based host–guest composites and paves the way for the broader implementation in solid-state optoelectronic applications. [ABSTRACT FROM AUTHOR]