Thiourea zinc sulfate (ZTS) crystal is a nonlinear optical material that has excellent performance, but the growthof ZTS crystal with high quality and large size is difficult. In this work, we calculated the dropping curve oftemperature in ZTS crystal growth and used the aqueous solution slow-cooling method to grow pure, Se dopedand As doped crystals. After the doping of Se/As, the external morphology and lattice parameters changed, andthe cell volume increased slightly. The decomposition temperature and hardness of Se/As doped crystals in-crease, indicating that thermostability and machinability are improved. The light transmittance of pure ZTS crystal is well and Se doped crystal is better, but As doped crystal is worse. The nonlinear optical property of ZTS crystal was studied by the powder frequency-doubling experiment.