Dielectric properties of (Mg (1¹x) Co x ) 4 Ta 2 O 9 (x = 0.01 to 0.09) prepared by solid state reaction were investigated. The maximum properties of the (Mg (1¹x) Co x ) 4 Ta 2 O 9 (x = 0.05) system were namely, an obtained ¾ r value of 12.27, a Q©f value of 440,000 GHz, and a¸f value of ¹59 ppm/°C sintered at 1325°C. The theoretical polarizability of (Mg (1¹x) Co x ) 4 Ta 2 O 9 increased with Co substitution, x. (Mg (1¹x) Co x ) 4 Ta 2 O 9 with Mg 2+ substituted by and Co 2+ not only improved the microwave dielectric properties, but also decreased sintering temperature. From the calculation of the covalency of cationoxygen bonds, it is found that the covalency of the CoO bond is lower than that of the MgO bond and the difference in the covalency between these cationoxygen bonds influences the temperature dependence of dielectric constant on the compounds. From our experiment, the best microwave dielectric property happens in (Mg 0.95 Co 0.05 ) 4 Ta 2 O 9 sintered at 1325°C for 4 h, and it's Q©f is 440,000 GHz with¸f = 59.5 ppm/°C.