Methylammonium (MA) lead hybrid perovskite single crystal recently received attention as a potential radiation detection material. Here, we report the MAPbBr 3 bulk crystals grown by the modified antisolvent vapor-assisted crystallization method. The growth rate is determined by diluting the antisolvent, which results in the average size of MAPbBr 3 crystals to significantly increase from 2 × 2 × 1 to 15 × 15 × 5 mm 3 . The morphology evolution of MAPbBr 3 crystals, which is contributed by the growth anisotropy, has been discussed according to the molar ratios of precursors and the bond theory. The resulting centimeter-sized MAPbBr 3 crystals exhibit high resistivity (5.6 × 10 8 Ω•cm) at room temperature. The mobility−lifetime (μτ) products are measured under 241 Am (5.48 MeV) α particles irradiation, with the values of 2.2 × 10 −4 and 4.2 × 10 −4 cm 2 /V for electrons and holes, respectively. Simultaneously, the electrons and holes mobility are estimated to be 24.6 and 59.7 cm 2 /(V•s), respectively, using the α-source-induced transient waveforms.