Structural features and microwave dielectric properties of (1−x)(Sr 0.3 Ca 0.427 Nd 0.182 )TiO 3−x SmAlO 3 (0.05 ≤ x ≤ 0.4) ceramics were investigated. X-ray diffraction patterns illustrated that solid solutions with the orthorhombic perovskite were shown to be formed in the ranges of 0.05 ≤ x ≤ 0.4. Moreover, the dielectric constant (ε r ) of sintered ceramics had a quasi-linear decrease with the increase in SmAlO 3 content. A certain amount of Sm and Al substitution for A-and B-sites could substantially improve the quality factor (Qf ) of the ceramics. Increasing the oxygen octahedral distortion led to a decrease in the temperature coefficient of the resonant frequency (τ f ) from 216.3 to −34.8 ppm • C −1 . Additionally, optimized microwave dielectric properties can be achieved for the specimens using 0.75(Sr 0.3 Ca 0.427 Nd 0.182 )TiO 3 -0.25SmAlO 3 ceramics [ε r ∼ 58.3, Qf ∼ 18800 GHz (at 4.65 GHz) and τ f ∼ 2.3 ppm • C −1 ] after being sintered at 1500 • C for 4 h. Keywords. (Sr 0.3 Ca 0.427 Nd 0.182 )TiO 3 ; SmAlO 3 ; microwave dielectric properties; oxygen octahedral distortion.