AbstractTo develop high‐performance piezo‐/ferroelectric materials, Bi(Zn_½Ti_½)O₃–PbZrO₃–PbTiO₃ (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 the yBi(Zn_½Ti_½)O₃–(1 − y)[(1 − x)PbZrO₃–xPbTiO₃] system 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/cm², 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 high‐power piezoelectric applications.