The microstructures and the microwave dielectric properties of 0.7(Sr y Ca 1-y )TiO 3 -0.3(Sm x Nd 1-x ) AlO 3 (7SCT-3SNA) ceramics system prepared by conventional solid-state route were investigated. X-ray powder diffraction results showed solid solutions with the perovskite structure were completely formed within the entire observation x range, and the unit cell volume of 0.7CaTiO 3 -0.3(Sm x Nd 1-x )AlO 3 (7CT-3SNA) ceramics decreased with increasing x value. The substitution of Nd 3? by Sm 3? could enhance the densification of 7CT-3SNA ceramics, and consequently improve the dielectric properties of the ceramics. When x = 0.75, specimens exhibited excellent microwave dielectric properties with e r * 44.52, Q 9 f value *40,110 and s f value *-1 ppm/°C . For further improving the microwave dielectric properties of the samples, Ca 2? in 0.7CaTiO 3 -0.3(Sm x Nd 1-x ) AlO 3 were partially substituted by Sr 2? . The results showed that the replacement of Ca 2? by Sr 2? effectively enhanced the densification of specimens. By optimizing the composition, the ceramics with y = 0.01 in 0.7(Sr y Ca 1-y ) TiO 3 -0.3(Sm 0.75 Nd 0.25 )AlO 3 (7SCT-3SNA) showed high relative density and dense and uniform microstructures as well as well-developed grain growth with superior microwave dielectric properties: e r * 45.38, Q 9 f value *41,730 and s f value *-0.2 ppm/°C.