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The electrostrain properties of bismuth ferrite–barium titanate (BF–BT)‐based ceramics can be well regulated; however, this often occurs at the cost of piezoelectricity, and their electrostrain‐temperature stability is poor. To address these problems, defect engineering has been utilized to enhance the comprehensive properties via the unequal substitution of Na+. In this study, 0.69BiFeO3–0.3BaTiO...