Low-temperature sintering of 0.375Pb(Ni1/3Nb2/3)O3–0.25PbZrO3–0.375PbTiO3 was investigated. Raw material powders of high-purity NiO, Nb2O5, PbO, TiO2, and ZrO2 were mixed and ground to 0.2 µm on average, calcined at 850 °C for 2 h to obtain pyrochlore-free calcined powder, ground again, and finally sintered at 925 °C for 4 h, without adding sintering additives. The sintered sample showed a relative density = 99%, an electromechanical coupling factor planar mode k p = 0.61, a piezoelectric constant d 33 = 600 pm/V, and a Curie temperature T c = 189 °C. Accordingly, a multilayered actuator with pure Ag internal electrodes was prepared using the calcined powder.