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In this work, calcium barium zirconate titanate piezoelectric ceramics 0.4Ba(Zr0.2Ti0.8)O3- 0.6(Ba0.7Ca0.3)TiO3((1−x)BZT-xBCT, abbreviated as x BCZT, x = 0.6) were prepared by conventional solid state reaction method. Different surfactant additives (SDS, CTAB, PEG, and Tris–HCl, respectively) were added to the ball milling process before sintering. Meanwhile, the temperature and dwelling time during the sintering process were also systematically investigated. Their effects on the microstructural, electrical, and piezoelectric properties of the modified ceramics were investigated. It was found that with the Tris–HCl surfactant, the dispersion of the 0.6 BCZT ceramics was the best, and the average particle size was ~82 nm. By using the SDS surfactant, the ceramics showed the highest relative density, i.e., 97%. For the ferroelectric performances, the largest coercive field (Ec = 5.39 kV/cm) was observed in the sample using the SDS surfactant when the sample was sintered at 1300 °C for 6 h. For the dielectric performances, the largest dielectric constant (ε) was found to be 35,366.9 for the sample using CTAB surfactant and sintered at 1300 °C for 4 h. We discovered that CTAB-modified ceramics sintered at 1290 °C for 2 h had the highest maximum polarization Ps = 24.975 kV/cm and remnant polarization Pr = 8.200 kV/cm and sintered at 1300 °C for 4 h produced the highest piezoelectric constant d33 and dielectric constant of 94 pC/N and 35,366.7, respectively. [ABSTRACT FROM AUTHOR]