AbstractScintillating materials that convert ionizing radiation into low‐energy photons hold great potential for radiation detection, nondestructive inspection, medical radiography, and space exploration. However, organic scintillators are characterized by low radioluminescence, while bulky inorganic scintillators are not suitable for the development of flexible detectors. Here, high‐resolution X‐ray imaging using solution‐processable lanthanide‐based metal–organic frameworks as microscale scintillators is demonstrated. Mechanistic studies suggest that lanthanide ions absorb X‐rays to generate high‐density molecular triplet excitons, and excited linkers subsequently sensitize lanthanide ions via nonradiative resonance energy transfer. Furthermore, the crystalline nature offers a delocalized electronic feature rather than isolated subunits, which enables direct trapping of charge carriers by lanthanide emitters. By controlling the concentration ratio between Tb3+and Eu3+ions, efficient and color‐tunable radioluminescence of lanthanide ions can be achieved. When coupled with elastic, transparent polymer matrices, these metal–organic framework‐based microscintillators allow the fabrication of flexible X‐ray detectors. Such detectors feature a detection limit of 23 nGy s−1, which is 240 times lower than the typical radiation dose for medical diagnosis. X‐ray imaging with resolution higher than 16.6 line pairs per millimeter is further demonstrated. These findings provide insight into the future design of hybrid scintillators for optoelectronics and X‐ray sensing and imaging.