X-ray detectors have attracted significant attention because they are widely used in applications such as computed tomography (CT), homeland security, and environmental monitoring. [1,2] In particular, there is an ever-increasing demand to invent better semiconductor material and device design to attain even higher sensitivity and lower manufacturing cost. [3,4] In the past decades, various traditional semiconductors have been studied for X-ray detection applications, like silicon (Si), [5] high-purity germanium (HP-Ge), [6] amorphous selenium (α-Se), [7] mercury iodide (HgI 2), [8] cadmium zinc telluride (CdZnTe), [9] and so on. Unfortunately, none of them is very ideal, more specifically, neither HP-Ge nor CdZnTe is costeffective; Si and CdZnTe require high working voltage; Si and α-Se have low X-ray absorption coefficient and large leakage current. Also, the CdZnTe, Si, and HP-Ge require very high growth temperature exceeding 500 °C, Hg and Cd are highly toxic. Recently, solution-processable organic-inorganic metal-halide perovskites have been demonstrated as a promising candidate for high performance X-ray detectors. They are advantageous in strong X-ray absorption, processable at low temperature, low-cost fabrication, and superior semiconducting properties like low defect density, large mobility-lifetime product (μτ), long carrier diffusion length, etc. Noticeably, the recently reported X-ray detectors based on 3D perovskites including MAPbI 3 [4,10-12] and CsFAMA [13] microcrystalline thin films or MAPbX 3 (X = Cl, Br, I and their mixture), [14-24] Cs x FA 1−x PbI 3 , [25] CsPbBr 3 , [26-29] and Cs 2 AgBiBr 6 [30-32] single crystals have realized high sensitivity with the highest up to 2.1 × 10 4 µC Gy air-1 cm-2 , significantly larger than the state-of-the-art α-Se X-ray detectors. [33] Unfortunately, the dark current is too high and as is the photocurrent drift in X-ray detectors made of these hybrid organic and inorganic 3D perovskites, and this is expected based on serious ion migration in the materials. Even worse, ionic migration is recognized as the main root cause for material decomposition and performance degradation in perovskite devices. In order to obtain perovskites with low ion migration, low-dimensional perovskite single crystals, like inchsized 0D MA 3 Bi 2 I 9 [34-37] and Cs 3 Bi 2 I 9 , [38-40] 2D Cs 2 TeI 6 [41] and (NH 4) 3 Bi 2 I 9 , [42] have been adventured first by our group and Low ionic migration is required for a semiconductor material to realize stable high-performance X-ray detection. In this work, successful controlled incorporation of not only methylammonium (MA +) and cesium (Cs +) cations, but also bromine (Br-) anions into the FAPbI 3 lattice to grow inch-sized stable perovskite single crystal (FAMACs SC) is reported. The smaller cations and anions, comparing to the original FA + and Ihelp release lattice stress so that the FAMACs SC shows lower ion migration, enhanced hardness, lower trap density, longer carrier lifetime and diffusion length, higher charge mobility and the...