Lead-based ferroelectric (FE) ceramics exhibit superior electromechanical properties; therefore, there has been an increased focus on developing new lead-based FE materials with high Curie temperature (Tc) and enhanced properties. The aim of this study was to investigate new compositions in the Pb(Mg1/3Nb2/3)O3–Pb(Yb1/2Nb1/2)O3–PbTiO3(PMN–PYbN–PT) system to enhance the electromechanical properties while increasing the Tc and lowering the sintering temperature. The 0.575[0.5PMN–0.5PYbN]–0.425PT composition at PMN/PYbN (50/50) mole ratio were prepared by reactive sintering PMNT and PYbNT powder mixtures at 950°–1200°C for 4 h. PMNT and PYbNT powders were calcined via the columbite method. Samples were prepared by cold isostatic pressing at 80 MPa. Dense and fully perovskite 0.575[0.5PMN–0.5PYbN]–0.425PT ceramics were fabricated at 975°C for 4 h, and these samples displayed a remnant polarization (Pr) of 32 μC/cm2, coercive field (Ec) of 17 kV/cm, and a piezoelectric charge coefficient (d33) of 475 pC/N. It is proposed that this ternary system can be tailored for various applications.