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Two-dimensional organic-inorganic hybrid perovskite materials are considered to have great potential for radiation detection due to their outstanding operational stability and excellent optoelectronic properties. However, most currently used single crystal (SC) growth methods impose strict requirements on growth conditions, and their potential effectiveness also faces significant challenges, especially for those perovskite systems with significant differences in solubility between raw materials and target products. In this study, a dynamic seed rotation method was developed to relieve the above dilemma. With the help of this method, centimeter-sized high-quality [(TMOD)2PbBr4]5·H2O (TMOD is thiomorpholine-1,1-dioxide) SCs were harvested. X-ray detectors based on the as-prepared SC exhibit a high sensitivity of 5.35 × 103 μC Gyair−1 cm−2 and a low detection limit of 3.1 nGyair s−1. We believe this strategy can also be applied to the preparation of other perovskite materials, paving the way for the application of high-quality optoelectronic devices.