The capability to detect radiation signal like X-rays and gamma-rays has been improved dramatically in recent years. [1,2] X-ray detection is very important because of its wide range of applications in medical imaging, industrial monitoring, national security, environmental protection and remediation, and science research. In particular, flat-panel X-ray detector array is now playing an important role in in modern medical, security verification, and industrial production. [3,4] Among the materials developed for X-ray detectors, amorphous selenium (a-Se) becomes the most classic semiconductor material for direct X-ray detection (X-rays directly convert into current signals), and it is suitable for X-ray imaging because of its easy deposition process on large-scale flat-panel digital readout circuits. [5,6] Unfortunately, the conversion efficiency of a-Se is limited due to its low X-ray absorbance, caused by its low atomic number (Z = 34), accompanied by small carrier mobility and lifetime product (μτ) value of ≈10 −7 cm 2 V −1 , which leads to its very low sensitivity (440 μC Gy air −1 cm −2) even under high operating electric field (15 000 V mm −1). [7] In addition to the a-Se, many other traditional semiconductors, such as Si, [8,9] TlBr, [10,11] PbI 2 , [12,13] Ge, [14,15] HgI 2 , [16,17] CdZnTe, [18,19] and PbO, [20,21] have been well studied, and among of them, especially CdZnTe, has shown potential applications in commercial X-ray detectors. However, most of these materials either possess very high dark current and low sensitivity, or suffer from needing high-temperature (exceeding 500 °C) and complex growth equipment, let alone their high toxicity (cadmium (Cd), thallium (Tl), lead (Pb), and mercury (Hg)). Accordingly, there are still some difficulties in preparing a large area X-ray absorber layer with excellent uniformity at low temperature, limiting their application to mammography. Therefore, recently, low-temperature, solution-synthesized 60 μm thick polycrystalline methylammonium lead iodide CH 3 NH 3 PbI 3 (MAPbI 3) perovskite films have been prepared to detect 8 keV low energy X-rays with high sensitivity, and X-ray imaging was demonstrated on a photovoltaic device. [22] Later, Huang's group achieved sensitive X-ray imaging by integrating MAPbBr 3 single crystals (SCs) on a silicon substrate. [23,24] Since then, X-ray detection using many Pb-based perovskites Lead-based (Pb) perovskite recently emerged as a promising photoelectric material for direct ionization radiation detection with outstanding performance. Unfortunately, its application is limited due to its toxicity caused by high Pb content, serious ion migration, poor crystallite quality, unsatisfactory reproducibility, high resistivity, and large fluctuation of electronic properties. Herein, a better substitute of lead-free inch-sized (34.3 mm × 34.3 mm × 13.1 mm) high-quality halide (CH 3 NH 3) 3 Bi 2 I 9 single crystal (MA 3 Bi 2 I 9 SC) is presented with higher resistivity, lower ion migration, and better stability. The coplanar detector ...