High-performance Pb-based piezoelectric materials, typified by PbZr 1-x Ti x O 3 (PZT), have a stranglehold of the worldwide marketplace for transducers, actuators, and sensors. 1 However, much endeavor has been devoted to find their alternatives since Pb imposes strong threats to environmental and human security. 2,3 Over the numerous Pb-free candidates, BNT-based ceramics have a unique superiority that Bi 3+ is configured with a similar electronic structure (long pair electrons 6s 2 ) with Pb 2+ , leading to the highly polarizable nature which is beneficial to potential application in actuators. 4,5 The good electromechanical response of BNT-based ceramics, which is directly related to their characteristic mesoscopic structures, is advantageous to their