ABSTRACT In this study, piezoelectric properties of 0.4Bi(Ni0.5Zr0.5)O3–0.6PbTiO3 (BNZ-PT) and 0.4Bi(Mg0.5Zr0.5)O3–0.6PbTiO3 (BMZ-PT) ceramics were investigated and compared with those of Pb(Zr,Ti)O3 in energy harvester applications. Their piezoelectric properties are comparable with those of Pb(Zr,Ti)O3 based materials, although they have lower lead contents. By optimizing the sintering temperature, the piezoelectric charge coefficients (d33) were improved to 438 and 351 pC/N for 0.4BNZ-0.6PT and 0.4BMZ-0.6PT, respectively, whereas the piezoelectric voltage coefficients (g33) were improved to 25.02 × 10−3∙V∙m/N and 28.37 × 10−3∙V∙m/N for 0.4BNZ-0.6PT and 0.4BMZ-0.6PT, respectively. The generated energies were estimated by measuring the generated output voltages. Generated energy densities of 1.67 and 1.01 mJ/cm3 were obtained from 0.4BNZ-0.6PT and 0.4BMZ-0.6PT, respectively. The optimum sintering conditions were found by observing the changes in the piezoelectric constant, dielectric constant, and density as a function of the sintering temperature.