Perovskite developments in the Pb(Zn1/3Ta2/3)O-3-PbTiO3 system were explored. Formation yields and lattice parameters of the perovskite were determined from X-ray diffractometry results. Weak-field low-frequency dielectric properties of the system ceramics were investigated, followed by microstructure examination. Perovskite started to develop in Pb(Zn1/3Ta2/3)O-3 after the introduction of 30 mol% PbTiO3, whereas complete stabilization was accomplished at 60% substitution. Dielectric relaxation behavior was not substantial across the entire composition range, whereas phase transition modes changed from diffuse to sharp with increased PbTiO3 fraction.