Abstract(1-x-y)BiFeO 3 -x(K 0.5 Bi 0.5 )TiO 3 -y PbTiO 3 piezoelectric ceramics were investigated across the compositional space and contrasted against the BiFeO 3 -(K 0.5 Bi 0.5 )TiO 3 system, a spectrum of relaxor-like/ferroelectric behavior was observed. Structural and piezoelectric properties were found to be closely related to the PbTiO 3 concentration, below a critical concentration, relaxor-type behavior was observed. The mechanisms governing the piezoelectric behavior were investigated with the use of a number of techniques including structural, electrical and imaging techniques. X-ray diffraction established that long-range crystallographic order was promoted above a critical PbTiO 3 concentration, y > 0.1125. Commensurate with the structural analysis, electric-field induced strain responses showed electrostrictive behavior in the PbTiO 3 -reduced compositions, with increased piezoelectric switching in PbTiO 3 -rich compositions. PUND analysis was used to confirm electric-field induced polarization measurements, elucidating that the addition of PbTiO 3 increased the switchable polarization and long-range ferroelectric ordering. PFM of the BiFeO 3 -(K 0.5 Bi 0.5 )TiO 3 -PbTiO 3 system exhibited typical domain patterns above a critical PbTiO 3 threshold, with no ferroelectric domains observed in the lead-free system in the pseudocubic region. Doping of BiFeO 3 -PbTiO 3 has been unsuccessful in the search for high-temperature materials that offer satisfactory piezoelectric properties, however, this system demonstrates that the partial substitution of alternative end-members can be an efficacious method. The partial substitution of PbTiO 3 into BiFeO 3 -(K 0.5 Bi 0.5 )TiO 3 enables long range crystallographic order, resulting in increased polar order and T C . The search for novel high-temperature piezoelectric ceramics can therefore exploit the accommodating nature of the perovskite family, which allows significant variance in chemical and physical character in the exploration of new solid-solutions.