Abstract The development of high-performance lead-free K0.5Na0.5NbO3-based piezoceramics for replacing commercial lead-containing counterparts is crucial for achieving environmentally sustainable society. Although the proposed new phase boundaries (NPB) can effectively improve the piezoelectricity of KNN-based ceramics, the difficulty of achieving saturated poling and the underlying multiscale structures resolution of their complex microstructures are urgent issues. Here, we employ a medium entropy strategy to design NPB and utilize texture engineering to induce crystal orientation. The developed K0.5Na0.5NbO3-based ceramics enjoys both prominent piezoelectric performance and satisfactory Curie temperature, thus exhibiting an ultrahigh energy harvesting performance as well as excellent transducer performance, which is highly competitive in both lead-free and lead-based piezoceramics. Comprehensive structural analysis have ascertained that the field-induced efficient multiscale polarization configurations irreversible transitions greatly encourages high saturated poling. This study demonstrates a strategy for designing high-performance piezoceramics and establishes a close correlation between the piezoelectricty and the underlying multiscale structures.
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