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In this study, LiF was utilized to decrease sintering temperature, improve microstructure, enhance Q × f , and regulate τ f of Li 2 Ti 0.9 (Zn 1/3 Ta 2/3) 0.1 O 3 (abbreviated as LTZT) ceramics. A complete solid solution together with a phase transition from monoclinic to cubic rock salt structure occurred. The cell volume of LTZT ceramics decreased as the LiF content increased. Relatively dense and uniform microstructures were observed for the ceramics as the LiF content was not less than 2 wt%. The dielectric constant of LTZT ceramics initially increased and then decreased with the increasing LiF content. The FWHM of the Raman band at about 808 cm−1 was closely related to the Q × f value. Notably, the samples with 3 wt% LiF exhibited the highest relative density of 97.4 % and satisfactory microwave dielectric properties of ε r = 23.14 ± 0.16, Q × f = 110,090 ± 1100 GHz, and τ f = +3.25 ± 1.45 ppm/°C when sintered at 950 °C. Good chemical compatibility with silver indicated the ceramic is a promising candidate in LTCC applications. [ABSTRACT FROM AUTHOR]