In this work, anisotropic LiNb0.6Ti0.5O3 (LNT) template particles are prepared by molten salt synthesis in LiCl flux. Plate‐like particles with diameters of 5–20 μm and
thicknesses of 0.5–2.0 μm synthesized at 1000°C are chosen as templates. Highly textured microwave ceramics of M‐phase LNT with tunable dielectric properties are fabricated by a novel screen‐printing templated grain growth technique (sp‐TGG),
and their characteristics and dielectric properties are studied systematically. Dielectric anisotropy is observed in dielectric constant (εr) and the temperature coefficient of dielectric constant (τε) at 1 MHz. LNT(//)
samples exhibit lower εr (=55.3) than randomly oriented ceramics and a positive temperature coefficient τε (75 ppm/°C), whereas, LNT(⊥) samples exhibit higher εr (=83.6) and a negative
temperature coefficient τε (= −120 ppm/°C). The textured ceramics also exhibit anisotropic and excellent properties at microwave frequency, with LNT‐M(//) showing εr = 57.9, Q × f = 6325 GHz,
τf= −14 ppm/°C and LNT‐M(⊥) showing εr = 81.8, Q × f = 5751 GHz, τf= 43 ppm/°C. By
tailoring along different directions, continuously tunable dielectric constant ranging from 55 to 83 could be obtained, and τf could be changed from −14 to 43 ppm/°C. These findings can be technologically beneficial for wireless communication devices.