In the present article, two kinds of metal-organic coordination compounds were synthesized between 4-mercaptopyridine (4-MPy) and nitrate of Ag(Ⅰ) and Cd(Ⅱ) by a general solution reaction and evaporation. 4-mercaptopyridine and two transition metal complexes were investigated by means of infrared, Raman and ultraviolet-visible spectroscopic techniques, respectively. Assignments of the main FTIR and Raman bands were carried out in detail. The relationship between those characteristic bands and the structure of ligands and coordination compounds was discussed. In the FTIR spectra, the co-vibration absorption band of ν(CC) and ν(CN), for 4-MPy at 1　459 cm-1 blue-shifted to 1　464 cm-1 for both the metal-organic coordination compounds, respectively. The Raman spectra, for the two coordination compounds, at 1　004 and 1　008 cm-1, which can be assigned to ring breathing vibration, at 1　617 and 1　615 cm-1, which can be assigned to ring flex vibration, and at 720 and 720 cm-1, which can be assigned to the composite vibration of β(C—C) and ν(C—S) are similar, respectively.