Metal halide perovskite materials, which combine outstanding physical properties, large absorption coefficient, tailored composition, and low-cost solution-processing, have aroused wide attention for use in various optoelectronic devices. Recently, perovskite single crystals have been rapidly outpacing traditional semiconductor materials in the field of radiation detection. As a prerequisite, achieving high-quality single crystals under controllable solution-phase growth must be tackled to fulfill their full potential as a new paradigm in this stagnated field. This Perspective summarizes the advances in X-ray detectors based on lead halide perovskite single crystals, presenting a comprehensive picture of the relationship among composition engineering, synthesis, and device properties. Additionally, we share our thoughts on several outstanding challenges of perovskite single crystals as promising X-ray detectors and propose possible approaches to the unresolved issues. We anticipate that this Perspective can open up new opportunities to improve their optoelectronic properties, which confers fascinating photonics applications with above and beyond state-of-the-art performance.