The La2O3–B2O3–ZnO (LBZ) glass was proved to be an effective sintering aid of the 0.45Ca0.6Nd0.26TiO3–0.55Li0.5Nd0.5TiO3 (CNT–LNT) ceramics. The influence of LBZ glass on the phase composition, low temperature sintering process, microstructure, activation energy, and dielectric properties of CNT–LNT ceramics was investigated in detail. The LBZ glass induced an obvious decrease of the CNT–LNT ceramics sintering temperature from 1350 to 1000 °C due to the liquid phase formation, which reduced the activation energy (Ea) of the CNT–LNT ceramics. In addition, the near zero temperature coefficient of resonant frequency (τƒ) value was obtained by adding moderate quantity of LBZ glass. CNT–LNT + 5 wt% LBZ (CNT–LNT + 5L) ceramics sintered at 1000°C/4 h displayed good microwave dielectric properties of: er = 101.7, Q × f = 1560 GHz (f = 3.25 GHz) and τƒ = 2.3 ppm °C−1.