Terahertz (THz) technology has immersing potential applications in industrial non-destructive testing, scientific research and military engineering. However, as the most commonly used THz emission and detection electro-optical material, the ZnTe single crystal growth still faces great challenges. In order to achieve ZnTe single crystals with large size, good homogeneity and high performance, an accelerated crucible rotation technique (ACRT) was introduced in growing ZnTe crystals by temperature gradient solution growth method (TGSG). Intrinsic ZnTe single crystals with high crystalline quality were successfully prepared. Through the simulation of flow field and solute distribution at different rotation speeds, the influence of ACRT technology on the stability of solid-liquid interface and Te inclusions distribution in crystal growth were investigated. During the crystal growth, the ACRT technology can effectively promote the melt flow, improve the solute mass transfer ability and stabilize the solid-liquid interface, which not only avoids the appearance of mixed phase zone at the crystal tail, but also reduces the number and size of Te inclusions in the crystal. With the further optimizing parameters, a large size ZnTe single crystal with a diameter of 60 mm was prepared. Meanwhile, the high response area of terahertz exceeding 90% faces due to the great uniformity of ZnTe crystal, which meant the edge effect being significantly limited and the ZnTe crystal meeting the commercial imaging requirements. Therefore, introduction of ACRT technology can provide a new strategy for preparation of ZnTe based electro-optical crystals.