Although perovskite wafers with a scalable size and thickness are suitable for direct X‐ray detection, polycrystalline perovskite wafers have drawbacks such as the high defect density, defective grain boundaries, and low crystallinity. Herein, PbI2‐DMSO powders are introduced into the MAPbI3 wafer to facilitate crystal growth. The PbI2 powders absorb a certain amount of DMSO to form the PbI2‐DMSO powders and PbI2‐DMSO is converted back into PbI2 under heating while releasing DMSO vapor. During isostatic pressing of the MAPbI3 wafer with the PbI2‐DMSO solid additive, the released DMSO vapor facilitates in situ growth in the MAPbI3 wafer with enhanced crystallinity and reduced defect density. A dense and compact MAPbI3 wafer with a high mobility‐lifetime (µτ) product of 8.70 × 10−4 cm2 V−1 is produced. The MAPbI3‐based direct X‐ray detector fabricated for demonstration shows a high sensitivity of 1.58 × 104 µC Gyair−1 cm−2 and a low detection limit of 410 nGyair s−1.