Ultrahigh Piezoelectric Properties in Textured (K,Na)NbO3‐Based Lead‐Free Ceramics

High‐performance lead‐free piezoelectric materials are in great demand for next‐generation electronic devices to meet the requirement of environmentally sustainable society. Here, ultrahigh piezoelectric properties with piezoelectric coefficients (d33 ≈700 pC N−1, d33* ≈980 pm V−1) and planar electromechanical coupling factor (kp ≈76%) are achieved in highly textured (K,Na)NbO3 (KNN)‐based ceramics. The excellent piezoelectric properties can be explained by the strong anisotropic feature, optimized engineered domain configuration in the textured ceramics, and facilitated polarization rotation induced by the intermediate phase. In addition, the nanodomain structures with decreased domain wall energy and increased domain wall mobility also contribute to the ultrahigh piezoelectric properties. This work not only demonstrates the tremendous potential of KNN‐based ceramics to replace lead‐based piezoelectrics but also provides a good strategy to design high‐performance piezoelectrics by controlling appropriate phase and crystallographic orientation. Textured (K,Na)NbO3‐based piezoelectric ceramics with ultrahigh piezoelectric properties (d33 ≈700 pC N−1, d33* ≈980 pm V−1, kp ≈76%) are prepared through a template grain growth method. The intrinsic piezoelectric anisotropy, large lattice distortion, the existence of intermediate monoclinic phase and nanodomain structure are considered likely to be responsible for the excellent piezoelectric properties. These results highlight the textured (K,Na)NbO3‐based lead‐free ceramics for piezoelectric device applications.