Lead-free (1-x-y)Na1/2Bi1/2TiO3-xBaTiO3-yBiFeO3 ceramics were synthesized by ordinary sintering technique. The compositional dependence of phase structure and electrical properties of the ceramics was systematically investigated. All samples possessed pure perovskite structure. The dielectric and piezoelectric properties of ceramics were investigated with the amount of different BiFeO3 substitutions. The addition of BiFeO3 can not only decrease Ec and Pr but also lead to a significant degradation of the dielectric loss tanδ.