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x mol% Fe‐doped Ba(Zr0.2Ti0.8)O3‐50 mol%(Ba0.7Ca0.3)TiO3 (abbreviated as xFe:BCZT) ferroelectric ceramics with x = 0, 0.075, 0.375, 0.75, 1.5, and 3 are fabricated via conventional solid‐state reaction methods. Fe incorporates into the lattice, and all the xFe:BCZT ceramics show pure perovskite structure except 3Fe:BCZT ceramics in which tiny amount of iron oxide is detected via X‐ray diffraction (XRD). The average grain sizes are significantly reduced from ≈20 to ≈2 μm with increasing Fe‐doping content. The Curie temperature of xFe:BCZT ceramics decreases with increasing Fe‐doping concentration and the room temperature dielectric constant significantly increased. Polarization hysteresis loops become slim after Fe‐doping. The recoverable energy storage density Wrec of xFe:BCZT ceramics is slightly enhanced to 0.240 J cm−3 with an energy storage efficiency η% = 70.1% at x = 0.075 under E‐field of 50 kV cm−1. The η% can be enhanced to as high as 93.8% at x = 3 with Wrec = 0.153 J cm−3 due to a slim P–E loops via Fe‐doping. The results indicate a potential method to fabricate high efficiency energy storage materials via Fe‐doping.

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