“…Piezoelectric materials, with the superior function of energy conversion from mechanical form to electrical form or vice versa, have found extensive applications in the fields of sensing, medical ultrasound imaging, underwater communication, and other fields. − Among all of the piezoelectric materials, the ferroelectric family shows the most superior piezoelectric response, thereby attracting numerous research interests. Although ferroelectric materials vary, the core functions have always been to enable devices with excellent performance outputs within a wide operational range in numerous electromechanical applications; therefore ferroelectric materials with high piezoelectric response and excellent stability are highly required, , flourishing research of exploring the origin of ultrahigh piezoelectricity and improving its piezoelectric performance as well as stability. − Numerous strategies have been proposed to acquire large piezoelectricity in ferroelectric materials, including the constructions of multiphase coexistence, polar nanoregions (PNRs), and electric-field-induced phase transition, etc. ,− Among them, Pb-based relaxor ferroelectric crystals have made remarkable progress in the design, research, and application of ultrahigh piezoelectricity. ,,, However, lead-free ferroelectrics with high performance and excellent stability are preferred over Pb-based materials due to environmental issues. Among all the lead-free ferroelectrics that are widely considered, the potassium sodium niobate ((K, Na)NbO 3 , KNN) family has drawn extensive attention owing to their high Curie temperature and excellent piezoelectric properties. ,− …”