To develop high-performance piezo-/ferroelectric materials, Bi(Zn ½ Ti ½ )O 3 -PbZrO 3 -PbTiO 3 (BZT-PZ-PT) ternary solid solution with compositions around the morphotropic phase boundary (MPB) is synthesized by solid-state reaction. The crystal structure and electric properties are investigated systematically by X-ray powder diffraction (XRD), dielectric spectroscopy, and ferroelectric and piezoelectric measurements. On the basis of the results of the XRD, dielectric and ferroelectric measurements, the pseudo-binary phase diagram of thesystem has been constructed for three series, namely, y = 0.05, 0.10, and 0.15. It is found that the introduction of BZT into the PZT system makes the paraelectric to ferroelectric phase transition more diffuse, brings the MPB to a lower PT content, and enlarges the MPB region. The best properties with an improved dielectric constant ε' = 1248, and a large remnant polarization P r = 33 μC/cm 2 , as well as a relatively high T C = 286 • C, and a high coercive field E c = 23 kV/cm was achieved in the y = 0.15 series with MPB composition x = 0.425, making it a promising material for highpower piezoelectric applications.