Abstract[001]C‐Textured 0.55Pb(Ni1/3Nb2/3)O3–0.15PbZrO3–0.3PbTiO3 (PNN‐PZT) ceramics are prepared by the templated grain‐growth method using BaTiO3 (BT) platelet templates. Samples with different template contents are fabricated and compared in terms of texture fraction, microstructure, and piezoelectric, ferroelectric and dielectric properties. High piezoelectric performance (d33 = 1210 pC N−1, d33* = 1773 pm V−1 at 5 kV cm−1) and high figure of merit g33⋅d33 (21.92 × 10−12 m2 N−1) are achieved in the [001]C‐textured PNN‐PZT ceramic with 2 vol% BaTiO3 template, for which the texture fraction is 82%. In addition, domain structures of textured PNN‐PZT ceramics are observed and analyzed, which provide clues to the origin of the giant piezoelectric and electromechanical coupling properties of PNN‐PZT ceramics.

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High-performance piezoelectrics are pivotal to various electronic applications including multilayer actuators, sensors, and energy harvesters. Despite the presence of high Lotgering factor F 001 , two key limitations to today's relaxor-PbTiO 3 textured ceramics are low piezoelectric properties relative to single crystals and high texture temperature. In this work, Pb(Yb 1/2 Nb 1/2 )O 3 -Pb(Mg 1/3 Nb 2/3 )O 3 -PbTiO 3 (PYN-PMN-PT) textured ceramics with F 001 ∼ 99% were synthesized at only 975 °C through liquid-phase-assisted templated grain growth, where of particular significance is that single-crystal properties, i.e., very large electrostrain S max /E max ∼ 1830 pm V −1 , giant piezoelectric figure of merit d 33 × g 33 ∼ 61.3 × 10 −12 m 2 N −1 , high electromechanical coupling k 33 ∼ 0.90, and Curie temperature T c ∼ 205 °C, were simultaneously achieved. Especially, the S max /E max and d 33 × g 33 values correspond to ∼180% enhancement as compared to the regularly 1200 °C-textured ceramics with F 001 ∼ 96%, representing the highest values ever reported on piezoceramics. Phase-field simulation revealed that grain misorientation has a stronger influence on piezoelectricity than texture fraction. The ultrahigh piezoelectric response achieved here is mainly attributed to effective control of grain orientation features and domain miniaturization. This work provides important guidelines for developing novel ceramics with significantly enhanced functional properties and low synthesis temperature in the future and can also greatly expand application fields of piezoceramics to high-performance, miniaturized electronic devices with multilayer structures.

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