Abstract: The redox characteristics of the ternary clathrate compound {Mo[S₂CN(C₂H₅)₂]₄}⁺{C₆H₅CH₂SSCH₂C₆H₅}^-was studied by electrochemical measurement and quantum-chemical calculations.The cyclic voltammogram of this ternary clathrate compound in 0.1M KClO₄-DMF with a platinum electride had 2.pairs of redox peak.Both the electrochemical parameters derived from the voltammogram and the results of EHMO calculations indicate that the pair of redox peak at relatively positive potentials corresponds to the redox reaction of Fe(Ⅲ)/Fe(Ⅱ) which is irreversible in nature,while the pair of redox peak at more negative potentials corresponds to the redox reaction of Mo(Ⅴ)/ Mo(Ⅱ) which is semi-reversible.The calculations from experiment measurements are fairly agreement with the theoretical calculations.