0.3Pb(Ni1/3Nb2/3)O3−xPbTiO3–(0.7−x)PbZrO3 (x=0.33–0.43) piezoelectric ceramics were prepared by the one-step solid-state reaction method. X-ray diffraction analysis showed the coexistence of rhombohedral and tetragonal phases at the composition x=0.39, which is the morphotropic phase boundary (MPB) for this system. The dielectric, ferroelectric, and piezoelectric properties of 0.3Pb(Ni1/3Nb2/3)O3–xPbTiO3–(0.7−x)PbZrO3 were investigated as a function of the content of PbTiO3. The ceramics at MPB showed large remnant polarization, low coercive field, and good piezoelectric properties. The results showed that piezoelectric ceramics with high piezoelectric constant and high Curie temperature also can be obtained in Pb(Ni1/3Nb2/3)O3–PbTiO3–PbZrO3 system with low Pb(Ni1/3Nb2/3)O3 content.