To develop high-performance materials for high-power piezoelectric applications, ternary high-density solid solutions with compositions of xPb(Zr0.52Ti0.48)O3− yPb(Mn1/3Sb2/3)O3−zPb(Zn1/3Nb2/3)O3 (PZTxPMSyPZnNz) with x = 0.82−0.96, y = 0.02−0.16, and z = 0.02−0.16, were fabricated by a conventional solid-state reaction method. A detailed investigation was carried out into the microstructure and crystal structure of the samples, together with their piezo-and ferroelectric properties. It was found that a solid solution with x = 0.86, y = 0.085, and z = 0.055 and a rhombohedral structure exhibited excellent piezo-and ferroelectric properties. These included piezoelectric coefficients d33 (longitudinal length mode) = 170 pC/N and -d31 (transverse length mode) = 69 pC/N, a mechanical quality factor Qm(p) (radial mode) = 2218, d33⋅Qm(p) = 376×10 3 pC/N, -d31⋅Qm(p) = 133×10 3 pC/N, electromechanical coupling factors kp (radial mode) = 46% and k31 (transverse length mode) = 28%, a Curie temperature Tc = 259°C, a remanent polarization 2Pr = 53 µC/cm 2 , and a coercive field 2Ec = 34 kV/cm. Thus, this is a highly promising piezoelectric material for high-power ultrasonic vibrators and piezoelectric transformers.