Relaxor-based piezoelectric single crystals of lead indium niobate-lead titanate (0.63Pb(In1/2Nb1/2)-0.37PbTiO3, abbreviated as PIN-PT), in the vicinity of the morphotropic phase boundary, were prepared by a flux method. The compositions of the flux, Pb3O4 or PbF2, play different role in perovskite stability and phase development. Thus, pure perovskite PIN-PT single crystals with the size of 2~5 mm were obtained by using Pb3O4 flux as well as a small amount of B2O3 additive. The microstructure and the phase development of the as-grown single crystals were investigated by scanning electron microscopy and transmission electron microscopy and X-ray diffraction. Furthermore, the dielectric properties of the <100>-oriented PIN-PT single crystals were measured in the temperature range between 20°C and 400°C.