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Defect engineering is a well‐established approach to customize the functionalities of perovskite oxides. In demanding high‐power applications of piezoelectric materials, acceptor doping serves as the state‐of‐the‐art hardening approach, but inevitably deteriorates the electromechanical properties. Here, a new hardening effect associated with isolated oxygen vacancies for achieving well‐balanced performances is proposed. Guided by theoretical design, a well‐balanced performance of mechanical quality factor (Qm) and piezoelectric coefficient (d33) is achieved in lead‐free potassium sodium niobate ceramics, where Qm increases by over 60% while d33 remains almost unchanged. By atomic‐scale Z‐contrast imaging, hysteresis measurement, and quantitative piezoresponse force microscopy analysis, it is revealed that the improved Qm results from the inhibition of both extrinsic and intrinsic losses while the unchanged d33 is associated with the polarization contributions being retained. More encouragingly, the hardening effect shows exceptional stability with increasing vibration velocity, offering potential in material design for practical high‐power applications such as pharmaceutical extraction and ultrasonic osteotomes.

Lead zirconate titanate [Pb(ZrxTi1−x)O3, PZT] thin films with various compositions, whose Zr/Ti ratio were varied as 40/60, 48/52, 47/53, and 60/40, were deposited on Pt(111)/Ti/SiO2/Si substrates by sol-gel method. A seeding layer was introduced between the PZT layer and the bottom electrode to control the texture of overlaid PZT thin films. A single perovskite PZT thin film with absolute (100) texture was obtained, when lead oxide was used as the seeding crystal, whereas titanium dioxide resulted in highly [111]-oriented PZT films. The dielectric and ferroelectric properties of PZT films with different preferential orientations were evaluated systemically as a function of composition. The maximums of relative dielectric constant were obtained in the morphotropic phase boundary region for both (100)- and (111)-textured PZT films. The ferroelectric properties also greatly depend on films’ texture and composition. The intrinsic and extrinsic contributions to dielectric and ferroelectric properties were discussed.