AbstractFlexible scintillator screens with excellent stability and low detection limits are crucial for X‐ray imaging applications. 0D organic metal halide materials have emerged as a strong contender in the scintillator fields, owing to their excellent optical characteristics and simple maneuverability. Herein, high‐quality and large quantities of C38H36P2Sb2Cl8 single crystals are synthesized through a simple solution approach. The prepared single crystals with dimer‐structure [Sb2Cl8]2− exhibit yellow emission with a near‐unity high photoluminescence quantum yield (PLQY) of 99.8%, and possess an exceptional light yield of 41300 photons MeV−1, and a detection limit as low as 45.6 nGyair s−1. On this basis, a large‐size and ultra‐flexible C38H36P2Sb2Cl8 scintillator utilized for X‐ray imaging is prepared by template assembled method, demonstrating a high spatial resolution of 8.15 lp mm−1. The prepared ultra‐flexible scintillator screen can achieve excellent X‐ray imaging even after multiple bending and stretching, which can also provide clear non‐planar X‐ray imaging for irregular objects. In addition, the scintillator shows excellent stability in light, heat, X‐ray irradiation, and water. These results not only expand the optoelectronic application field of organic‐inorganic hybrid antimony halides but also promote the rapid development of efficient ultra‐flexible scintillators.