High‐Performance [001]c‐Textured PNN‐PZT Relaxor Ferroelectric Ceramics for Electromechanical Coupling Devices

[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. Texture engineering can enhance the electromechanical coupling performance compared to ordinary ceramics. [001]C‐textured 0.55Pb(Ni1/3Nb2/3)O3–0.15PbZrO3–0.3PbTiO3 (PNN‐PZT) ceramics are prepared using BaTiO3 platelet templates. Outstanding piezoelectric performance and high figure of merit g33⋅d33 are achieved at 2 vol% BaTiO3. The d33 of the PNN‐PZT‐textured ceramics exhibits the highest value ever reported in textured ceramics to date.