In this study, lead‐free (1 − x)Ba(Zr0.2Ti0.8)O3 − x(Ba0.7Ca0.3)TiO3 compositions are synthesized via conventional solid oxide route, and the ceramics are fabricated with normal sintering in air. The effects of composition fluctuations on dielectric, piezoelectric, and mechanical properties are investigated. The phase structure and the microstructure are analyzed with X‐ray diffraction and scanning electron microscopy. The best dielectric and piezoelectric properties of εr = 11 207 and d33 = 330 pC/N were obtained for BZT−0.35BCT and BZT−0.5BCT ceramics, respectively. The mechanical behavior—in terms of Vickers hardness and compressive and flexural strengths—was investigated, and the best mechanical behavior was found in the vicinity of the phase transition boundary with x values between 0.5 and 0.6.