Barium titanate (BaTiO 3) are functional ceramics with attractive ferroelectric and piezoelectric properties, 1-3 which enable their broad applications such as acoustic imaging, chip capacitors, and dynamic access memories. 4,5 The phase transformation of BaTiO 3 occurs with the temperatures: rhombohedral to orthorhombic at ~−90°C, orthorhombic to tetragonal at ~0°C, tetragonal to cubic at ~120°C, and cubic to hexagonal at ~1460 o C. 6-8 Among these five polymorphs, tetragonal (t-BaTiO 3) phase is used to prepare piezoelectric ceramics with high piezoelectric coefficients and dielectric constants (d 33 ~ 1500 to 500 pC/N, and ε′ ~ 3000 to 6800 at a frequency range from 0.1 to 10 kHz, 25ºC). 9-11 In contrast, hexagonal BaTiO 3 (h-BaTiO 3) is a high-temperature phase that is usually metastable at room temperature. Li et al suggested that the hexagonal phase can be stabilized at room temperature via the substitution of Cr and Sb for Ti. 12 Regarding the dielectric properties, Akishige et al reported that single-crystal h-BaTiO 3 grown from the molten phase had a low dielectric constant (ε′ < 2200 at 1 kHz). 13 Later, Yu et al synthesized h-BaTiO 3 crystals using a pressurized