LAUSR

Piezoelectric materials enable the conversion of mechanical energy into electrical energy and vice‐versa. Ultrahigh piezoelectricity has been only observed in single crystals. Realization of piezoelectric ceramics with longitudinal piezoelectric constant (d33) close to 2000 pC N–1, which combines single crystal‐like high properties and ceramic‐like cost effectiveness, large‐scale manufacturing, and machinability will be a milestone in advancement of piezoelectric ceramic materials. Here, guided by phenomenological models and phase‐field simulations that provide conditions for flattening the energy landscape of polarization, a synergistic design strategy is demonstrated that exploits compositionally driven local structural heterogeneity and microstructural grain orientation/texturing to provide record piezoelectricity in ceramics. This strategy is demonstrated on [001]PC‐textured and Eu3+‐doped Pb(Mg1/3Nb2/3)O3‐PbTiO3 (PMN‐PT) ceramics that exhibit the highest piezoelectric coefficient (small‐signal d33 of up to 1950 pC N–1 and large‐signal d33* of ≈2100 pm V–1) among all the reported piezoelectric ceramics. Extensive characterization conducted using high‐resolution microscopy and diffraction techniques in conjunction with the computational models reveals the underlying mechanisms governing the piezoelectric performance. Further, the impact of losses on the electromechanical coupling is identified, which plays major role in suppressing the percentage of piezoelectricity enhancement, and the fundamental understanding of loss in this study sheds light on further enhancement of piezoelectricity. These results on cost‐effective and record performance piezoelectric ceramics will launch a new generation of piezoelectric applications.