Antiferroelectrics (AFEs) are promising candidates in energy-storage capacitors, electrocaloric solid-cooling, and displacement transducers. As an actively studied lead-free antiferroelectric (AFE) material, NaNbO3 has long suffered from its ferroelectric (FE)-like polarization-electric field (P-E) hysteresis loops with high remnant polarization and large hysteresis. Guided by theoretical calculations, a new strategy of reducing the oxygen octahedral tilting angle is proposed to stabilize the AFE P phase (Space group Pbma) of NaNbO3. To validate this, we judiciously introduced CaHfO3 with a low Goldschmidt tolerance factor and AgNbO3 with a low electronegativity difference into NaNbO3, the decreased cation displacements and [BO6] octahedral tilting angles were confirmed by Synchrotron X-ray powder diffraction and aberration-corrected scanning transmission electron microscopy. Of particular importance is that the 0.75NaNbO3−0.20AgNbO3−0.05CaHfO3 ceramic exhibits highly reversible phase transition between the AFE and FE states, showing well-defined double P-E loops and sprout-shaped strain-electric field curves with reduced hysteresis, low remnant polarization, high AFE-FE phase transition field, and zero negative strain. Our work provides a new strategy for designing NaNbO3-based AFE material with well-defined double P-E loops, which can also be extended to discover a variety of new lead-free AFEs.

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