Lead-free piezoelectric ceramics based on chiBi(Zn1/2Ti1/2)O3-(1-chi)(Bi1/2K1/2)TiO3 were obtained via solid state processing techniques. A single perovskite phase with tetragonal symmetry was obtained for Bi(Zn1/2Ti1/2)O3 (BZT) substitutions up to 20 mol%. The maximum density was 97.1% at the composition of chi = 0.1. The dielectric measurement indicated that the transition temperature decreased linearly with increasing BZT content. The P-E loops revealed an increase in remanent polarization (Pr) with the addition of BZT. The maximum planar coupling coefficient, kappar, for the chi = 0.1 composition was 21.6 and the piezoelectric coefficient, d33, for chi = 0, chi = 0.05, and chi = 0.1 was 108, 185, and 235 pm/V, respectively. Overall, the dielectric and piezoelectric properties showed significant improvement when BZT was added.