(1-x)Ba(Zr0.2Ti0.8)O3-(x)(Ba0.7Ca0.3)TiO3 ceramics where x = 0.3, 0.4, 0.5 and 0.6 were prepared employing a solid state sintering technique. X-ray diffraction patterns suggested a morphotropic phase boundary of rhombohedral and tetragonal structure. Upon increase of (Ba0.7Ca0.3)TiO3, the average grain size became smaller. The decrease of the phase transition temperature was observed in correlation with the (Ba0.7Ca0.3)TiO3 content. The coexistence of rhombohedral and tetragonal played an important role in enhancement of dielectric and piezoelectric properties. The result here suggested that electrical properties of these ceramics may be largely tunable and could be an attractive material for high-dielectric response and piezoelectric devices.