In this work, 0.73Li2ZnTi3O8–0.27Li2TiO3 ceramics were prepared through a traditional solid-state process. The effects of Li2O–B2O3–SiO2–CaO–Al2O3 (LBSCA) glass addition on phase formation, microstructure, sintering characteristic and microwave dielectric properties of the ceramics were investigated. A small amount of LBSCA glass addition significantly reduced sintering temperature of the ceramics. X-ray diffraction analysis revealed that Li2ZnTi3O8 and Li2TiO3 phases coexisted without producing any other crystal phases in the sintered ceramics. Dielectric constant and Qf values were related to the amount of LBSCA addition and sintering temperatures. The specimens obtained near-zero temperature coefficient (τf) values through the compensation on the positive τf of Li2TiO3 and the negative τf of Li2ZnTi3O8. The 0.73Li2ZnTi3O8–0.27Li2TiO3 ceramic with 0.75 wt% LBSCA addition and sintered at 900 °C for 3 h exhibited excellent microwave dielectric properties of ɛr = 23.907, Qf = 63050 GHz and τf = 1.2 ppm/°C, which was very suitable for LTCC (low temperature co-fired ceramics) applications.