High‐quality perovskite single crystals with large size are highly desirable for the fundamental research and high energy detection application. Here, a simple and convenient solution method, featuring continuous‐mass transport process (CMTP) by a steady self‐supply way, is shown to keep the growth of semiconductor single crystals continuously stable at a constant growth rate until an expected crystal size is achieved. A significantly reduced full width at half‐maximum (36 arcsec) of the (400) plane from the X‐ray rocking curve indicates a low angular dislocation of 6.8 × 106 cm−2 and hence a higher crystalline quality for the CH3NH3PbI3(MAPbI3) single crystals grown by CMTP as compared to the conventional inverse temperature crystallization (ITC) method. Furthermore, the CMTP‐based single crystals have lower trap density, reduced by nearly 200% to 4.5 × 109 cm−3, higher mobility increased by 187% to 150.2 cm2 V−1 s−1, and higher mobility–lifetime product increased by around 450% to 1.6 × 10−3 cm2 V−1, as compared with the ITC‐grown reference sample. The high performance of the CMTP‐based MAPbI3 X‐ray detector is comparable to that of a traditional high‐quality CdZnTe device, indicating the CMTP method as being a cost‐efficient strategy for high‐quality electronic‐grade semiconductor single crystals.

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