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The effect of calcination process on a phase evolution, a microstructure development and the piezoelectric properties were investigated in 0.75BiFeO 3 -0.25BaTiO 3 (0.75BF-0.25BT) ceramics. At the relatively low calcination temperatures of 600 °C–650 °C, a Bi 25 FeO 40 impurity phase was formed in addition to some unreacted raw materials and a perovskite phase. As the calcination temperature increased to the range of 700–900 °C, other intermediate phase BaBi 4 Ti 4 O 15 was formed concurrently with small amounts of unreacted BaCO 3 and perovskite matrix phase. At 950 °C a pure single perovskite phase of 0.75BF-0.25BT solid solution was observed. The sintered samples produced by using the raw powder calcined at a relatively low temperature of 600–900 °C showed a large fraction of pseudo-cubic relaxor phase (0.54–0.71 mass fraction) with the rest of a rhombohedral ferroelectric phase. They showed poor piezoelectric properties at sintering temperature below 1000 °C due to the nonuniform compositional distribution of the calcined powder. The homogeneous calcination at 950 °C for 2 h reduced greatly the optimum sintering temperature and significantly enhanced piezoelectric properties in the BF-BT ceramics. High Curie temperature as well as high piezoelectric properties were obtained at the sintering temperature as low as 920 °C: k p = 0.361, d 33 = 123 pC/N and T C = 653 °C in the 0.75BF-0.25BT ceramics and k p = 0.337, d 33 = 183 pC/N and T C = 525 °C in the 0.7BF-0.3BT ceramics. This low temperature sintering of the BF-BT ceramics by a homogeneous calcination could be applied to the fabrication of the lead-free multi-layer piezoelectric devices with inexpensive internal electrodes. [ABSTRACT FROM AUTHOR]