The solid solution crystal Pb(Zn1/3Nb2/3)O3-PbTiO3 [PZNT] has been grown from the high temperature solution. The crystallization behavior of PZNT was investigated. The evaporation of PbO was controlled by sealing crucible and the erosion of the melt or solution on Pt crucible was discussed. By optimizing growth conditions, high quality PZNT crystal was obtained. The ferroelectric properties were measured and the results showed as–grown crystal has high performance.