To meet the increasing demands for developing miniaturized high-precision modern piezoelectric devices, researchers are focusing their attention on PbTiO3 (PT) relaxor ferroelectrics having excellent comprehensive performance. Although the partial substitution of Pb(Mg1/3Nb2/3)O3 (PMN)-PT with Pb(Ni1/3Nb2/3)O3 (PNN)-PT has been reported to improve dielectric and piezoelectric properties, the factors underlying the performance improvement of the PNN-PMN-PT ternary system remain unclear. Therefore, based on PT content regulation, the 0.128PNN-(0.872-x)PMN-xPT (x = 0.316, 0.326, 0.336, 0.346, and 0.356) ternary ceramics were fabricated, and the crystal structure and electrical properties were systematically investigated during the rhombohedral-tetragonal phase transition. The 0.128PNN-0.536PMN-0.336PT composition exhibited optimum performance with the piezoelectric charge coefficient, effective piezoelectric strain coefficient, dielectric constant were 691 pC/N, 1060 pm/V and 4545 respectively at a maximum permittivity temperature of 136 ℃, signifying its potential for use in transducers and actuators. The outstanding properties of this system were mainly derived from the lattice distortion and reversible domain wall motion. The results indicated that the multiphase coexistence and enhanced B-site disorder in the perovskite structure contribute to the improvement in the piezoelectric properties, which would facilitate the design and development of novel piezoelectric materials.