With further substitution of Sn, the lattice constant, volume and apparent density of the ceramics increased, the ceramic structure reached a maximal compactness at x = 0.2 which was shown on SEM. Tremendous improvement of Q × f and a declining trend of r and τ f were obtained with increasing x value. Appropriate substitution value (x = 0.10) would ensure excellent microwave dielectric properties ( r = 34.1, Q × f = 40562 GHz, τ f = −5 ppm/°C) of the ceramics sintered at 1080°C.