The ternary system of lead nickel niobate Pb(Ni1/3Nb2/3)O3 (PNN), lead zinc niobate Pb(Zn1/3Nb2/3)O3 (PZN), and lead zirconate titanate Pb(Zr1/2Ti1/2)O3 (PZT) was investigated to determine the influence of different solid state processing conditions on dielectric and ferroelectric properties. The ceramic materials were characterized using x-ray diffraction, dielectric measurements, and hysteresis measurements. To stabilize the perovskite phase, the columbite route was utilized with a double crucible technique and excess PbO. The phase-pure perovskite phase of PNN–PZN–PZT ceramics was obtained over a wide compositional range. It was observed that for the ternary system 0.5PNN–(0.5 - x)PZN–xPZT, the change in the transition temperature (Tm) is approximately linear with respect to the PZT content in the range x[H11505] 0 to 0.5. With an increase in x, Tm shifts up to high temperatures. Examination of the remanent polarization (Pr) revealed a significant increase with increasing x. In addition, the relative permittivity ([H9280]r) increased as a function of x. The highest permittivities ([H9280]r [H11505] 22,000) and the highest remanent polarization (Pr [H11505] 25 μC/cm2) were recorded for the binary composition 0.5Pb(Ni1/3Nb2/3)O3–0.5Pb(Zr1/2Ti1/2)O3.