xSm(Mg 0.5 Ti 0.5 )O 3 -(1 -x)Ca 0.8 Sr 0.2 TiO 3 (x = 0.50-0.95) ceramics are prepared by a conventional solidstate ceramic route. The microstructure and microwave dielectric properties are investigated as a function of the x-value and sintering temperature. The single phase solid solutions were obtained throughout the studied compositional range. The variation of bulk density and dielectric properties are related with the x-value. Increasing sintering temperature can effectively promote the densification and dielectric properties of xSm(Mg 0.5 Ti 0.5 )O 3 -(1 -x)Ca 0.8 Sr 0.2 TiO 3 ceramic system. With the content of Sm(Mg 0.5 Ti 0.5 )O 3 increasing, the temperature coefficient of resonant frequency s f value decreased, and a near-zero s f could be obtained for the samples with x = 0.80. The optimal microwave dielectric properties with a dielectric constant e r of 30.1, Q 9 f of 115,000 GHz (at 8.0 GHz), and s f of 8.9 ppm/°C were obtained for 0.80Sm(Mg 0.5 Ti 0.5 )O 3 -0.20Ca 0.8 Sr 0.2 TiO 3 sintered at 1,550°C for 3 h, which showed high density and well-developed grain growth.