A new Bi-based (Bi0.5Na0.5)TiO3-based lead-free piezoelectric ceramics with perovskite structure, (1-x-y)BNT–xBKT– yBiFeO3, was prepared by a conventional ceramic sintering technique. The relation between composition and dielectric properties and the relation between composition and frequency were investigated. It was found that the dielectric constant and dielectric loss of unpoled samples is higher that those of poled samples. The dielectric properties of unpoled samples varied insignificant with the increase content of BiFeO3 and those of poled samples increased with the increase content of BiFeO3. The dielectric constant and dielectric loss of unpoled and poled samples increased with the increase content of BKT. The dielectric constant decreased and dielectric loss increased with increasing frequency, and the increase and decrease trend became slowly with increasing frequency.