Li2TiO3 ceramics were prepared at the sintering temperatures from 1050 to 1250 °C. The optimal microwave dielectric properties were ɛr = 23.29, Q × f = 15,525 GHz (5.9 GHz), and τf = 35.05 ppm/ °C for the sample sintered at 1200 °C. The microwave dielectric properties were improved obviously when the Li2TiO3 ceramics were sintered at low temperatures with small additions of H3BO3 (B2O3 in the form of H3BO3). Only monoclinic Li2TiO3 was found in the pure or H3BO3-doped Li2TiO3 ceramics. About 1.0 wt.% H3BO3 addition aided the sintering of Li2TiO3 ceramics effectively while excessive H3BO3 (≥2.5 wt.%) was not favorable. Typically the best microwave dielectric properties were ɛr = 23.28, Q × f = 37,110 GHz (6.3 GHz), and τf = 30.43 ppm/ °C for the 1.0 wt.% H3BO3-doped Li2TiO3 ceramic sintered at 920 for 3 h, which is promising for LTCC applications.