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Current powder–polymer composite scintillator films typically require thicknesses of hundreds of micrometers to millimeters to ensure sufficient X-ray attenuation and brightness. However, intrinsic particle aggregation and interfacial heterogeneity inevitably induce severe light scattering, thereby compromising spatial resolution. Herein, we develop two optically homogeneous hybrid metal halide glasses, MTP2SbCl5 and MTP2MnCl4 (MTP = methyltriphenylphosphonium), via a scalable low-temperature melt quenching strategy. These glasses exhibit high visible–near-infrared transmittance up to ~90% and excellent glass-forming ability. At a thickness of 1 mm, they deliver near-complete attenuation of X-rays (> 99.8%) and intense radioluminescence with light yields of 5819 and 19,232 photons·MeV−1, respectively. As a result, the glassy scintillators exhibit robust irradiation durability and achieve spatial resolutions of 18.8 and 22.5 lp·mm−1, respectively, representing a substantial twofold improvement over previously reported crystalline counterparts. Impressively, they possess a stimulus-responsive reversible glass–crystal transition, low-temperature self-healing, and tunable radioluminescence from green to orange–red via compositional engineering. These features not only overcome the scattering and monochromatic-emission limitations of traditional scintillators but also establish a novel paradigm for next-generation recyclable materials and multicolor radiation visualization platforms.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, http://creativecommons.org/licenses/by/4.0/).
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