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Abstract Quasi-two-dimensional (Q-2D) perovskite exhibits exceptional photoelectric properties and demonstrates reduced ion migration compared to 3D perovskite, making it a promising material for the fabrication of highly sensitive and stable X-ray detectors. However, achieving high-quality perovskite films with sufficient thickness for efficient X-ray absorption remains challenging. Herein, we present a novel approach to regulate the growth of Q-2D perovskite crystals in a mixed atmosphere comprising methylamine (CH3NH2, MA) and ammonia (NH3), resulting in the successful fabrication of high-quality films with a thickness of hundreds of micrometers. Subsequently, we build a heterojunction X-ray detector by incorporating the perovskite layer with titanium dioxide (TiO2). The precise regulation of perovskite crystal growth and the meticulous design of the device structure synergistically enhance the resistivity and carrier transport properties of the X-ray detector, resulting in an ultrahigh sensitivity (29721.4 μC Gyair −1 cm−2) for low-dimensional perovskite X-ray detectors and a low detection limit of 20.9 nGyair s−1. We have further demonstrated a flat panel X-ray imager (FPXI) showing a high spatial resolution of 3.6 lp mm−1 and outstanding X-ray imaging capability under low X-ray doses. This work presents an effective methodology for achieving high-performance Q-2D perovskite FPXIs that holds great promise for various applications in imaging technology.