Abstract
ABSTRACT
Solution‐processed scintillators are attractive for large‐area X‐ray imaging. However, their performance in thin‐film architectures is constrained by low effective density, severe light scattering, and insufficient thermal stability. Here, we report a solution‐processed epitaxial growth strategy to fabricate large‐area, monolithic metal–organic framework (MOF) thin‐film scintillators for temperature‐adaptive, high‐resolution X‐ray imaging. Mechanistic investigation reveals that surface hydroxyl‐mediated, molecularly oriented epitaxial growth reconstructs the interfacial energy landscape, enabling optically continuous, densely packed terbium–terephthalate (Tb‐BDC) films on solid substrates. The Tb‐BDC scintillator demonstrates a light yield of 44,380 photons MeV
−1
and exceptional thermal stability in scintillation performance. At 513 K, it retains 95.2% of its room‐temperature radioluminescence intensity, surpassing the 42.6% retained by commercial Gd
2
O
2
S:Tb. Furthermore, it maintains 93.7% of its initial radioluminescence intensity following cumulative X‐ray irradiation up to 67.4 Gy. Notably, its radioluminescence intensity remains within 3.6% of the pristine value after 24 h immersion in water. By integrating self‐supervised machine learning‐assisted image reconstruction, temperature‐adaptive X‐ray imaging with a spatial resolution of 21.7 lp mm
−1
is achieved. This work establishes an epitaxial microstructural design paradigm for solution‐processed scintillator screens operating under demanding thermal conditions.