Complex ferroelectric PbTiO3-modified 0.5Ba(Zr0.2Ti0.8)O3-0.5(Ba0.7Ca0.3)TiO3 materials were synthesized by a conventional solid-state reaction method. The addition of PbTiO3 into host 0.5Ba(Zr0.2Ti0.8)O3-0.5(Ba0.7Ca0.3)TiO3 materials are modified the ferroelectric properties of host materials where the maximum polarization slightly increased from 23.09 C\cm2 to 23.28 C\cm2 and the remnant polarization is found to increase from 10.07 C\cm2 to 11.31 C\cm2. The large piezoelectric dynamic coefficient value of 662 pm\V is obtained for 7 mol. % PbTiO3 modified 0.5Ba(Zr0.2Ti0.8)O3-0.5(Ba0.7Ca0.3)TiO3 compounds as solid solution. Our work is expected to contribute to the role of A-site modification in lead-free ferroelectric BaTiO3-based materials for advanced function materials for electronic device applications.