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Highlights The solution limit of manganese ion in BiFeO3–BaTiO3 (BF–BT) was determined by combining multiple advanced characterization methods. The defect engineering associated with fine doping can realize the co-modulation of polarization configuration, iron oxidation state and domain orientation. The BF–BT–0.2Mn piezoelectric energy harvester shows excellent power generation capacity at 250 °C, which is an important breakthrough for lead-free piezoelectric devices.