Abstract: Hydrothermal reaction of 1-methyl-1H-imidazole-4，5-dicarbonitrile （MID） and NaN₃ in the presence of Lewis acid transition metals sulfate （M = Fe^Ⅱ， Co^Ⅱ） afforded two coordination compounds Fe（MTIC）（H₂O） （1） Co（MTIC）（H₂O） （2） and a ligand structure （MTIC）（H₂O） （3）. The research indicated that only one of the cyano groups changed into tetrazolyl group through the Sharpless reaction while the other didn’t. X-ray diffraction analysis reveals that compounds 1-3 are mononuclear structure and crystallize in the same P-1 space group. In additional， all the complexes have been characterized by elemental analysis， thermal analysis， infrared spectra，and X-ray powder diffractometer. The research will provide a guidance and reference for exploiting new organic metal super-molecules materials.