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The 0.72Bi(Fe1−xAlx)O3–0.28BaTiO3 (x = 0, 0.01, 0.03, 0.05, and 0.07, abbreviated as BFAx–BT) lead‐free high‐temperature ceramics were prepared by the conventional ceramic processing. Systematic investigation on the microstructures, crystalline structures, dielectric and piezoelectric properties, and high‐temperature stability of piezoelectric properties was carried out. The crystalline structures of BFAx–BT ceramics evolve from rhombohedral structure with x < 0.01 to the coexistence of rhombohedral structure and pseudocubic phases with x ≈ 0.01, finally to pseudocubic phases when x > 0.03. Remarkably high‐temperature stability with near‐zero temperature coefficient of piezoelectric properties (TCkp), together with improved piezoelectric properties has been achieved for x = 0.01 BFAx–BT ceramics. The BFAx–BT(x = 0.01) ceramics simultaneously show the excellent piezoelectric properties of d33 = 151 pC/N, kp = 0.31 and super‐high‐temperature stability of Td = 420°C, TCkp = 1 × 10−4. It is considered that the observed strong piezoelectricity and remarkably high‐temperature stability should be ascribed to the phase coexistence of rhombohedral and pseudocubic phases. The rhombohedral phases have a positive TCkp value and the pseudocubic phases possess a negative TCkp value. Thus, the TCkp value of BFAx–BT ceramics can be tuned by composition of x.

Lead-free 0.985(0.96KNNT–0.04BNKZ)–0.015CZ ceramics were sintered at 1150–1190 °C.

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