for piezoelectric devices was estimated to be worth $25.1 billion with a projected compounded annual growth rate (CAGR) of 6.2%. [6] However, the development of piezoelectrics took more than a century to evolve from quartz, which is among the first known piezoelectric materials, [7,8] to their current forms in the modern era. The evolution of piezoelectrics is, hence, rich with the exciting discoveries in fundamental physics, paving the way to the development of applications that changed the course of history. One such example is the invention of sonar by Paul Langevin and team in 1917 [9] which is still essentially implemented today for underwater acoustics and navigation. Later, the discovery of ferroelectricity in BaTiO 3 polycrystal in 1946 [10,11] and phase transition (now referred to as a morphotropic phase boundary (MPB)) in PbZrO 3 -PbTiO 3 solid solution in 1954 [12] stimulated a worldwide interest in gaining fundamental understanding of electromechanical coupling in ferroelectric materials to develop better and more reliable piezoelectric devices. [13][14][15] By contrast, the research on piezoelectrics in the past two decades has been driven mainly by the environmental and health concerns related to the toxicity of lead, which is a primary constituent of the widely used lead-based piezoelectric ceramics, [16,17] where the best known example is lead zirconium titanates (PZT). Consequently, the stringent regulations all over the world to restrict the use of lead [18] have resulted in the rise of "lead-free" ceramics which further gained popularity after Saito et al.'s discovery of large piezoelectric response in a lead-free piezoceramic. [19] These eco-friendly materials represent now although a relatively small part of the current piezoelectrics market, with a total estimate of around $172 million, but, their sales are projected to reach $443 million by 2024 with a CAGR of 20.8%. [6] ABO 3 -type perovskite oxide ferroelectrics hold great technical value owing to their large spontaneous polarization, which makes them highly suitable for piezoelectric applications. [1,3,20] In recent years, the research efforts have been primarily focused on developing new strategies to produce high-performance lead-free oxide piezoelectrics with properties at least comparable to or surpassing those of the lead-based counterparts, such as PZT. [20] These strategies have mainly Piezoelectric materials are known to mankind for more than a century, with numerous advancements made in both scientific understandings and practical applications. In the last two decades, in particular, the research on piezoelectrics has largely been driven by the constantly changing technological demand, and the drive toward a sustainable society. Hence, environmental-friendly "lead-free piezoelectrics" have emerged in the anticipation of replacing lead-based counterparts with at least comparable performance. However, there are still obstacles to be overcome for realizing this objective, while the efforts in this direction already seem to culminat...