The reaction of [Cp*RuCl2](2) (1; Cp* = eta(5)-C5Me5) with tetraalkyldithiuram disulfides (R2NC(S)SS(S)CNR2, R = Me, Et), isopropylxanthic disulfide ([(PrOC)-Pr-i(S)S](2)), and bis(thiophosphoryl) disulfide ([((PrO)-Pr-i)(2)P(S)S](2)) led to the isolation of dark-red crystalline solids of Cp*(RuCl2)-Cl-IV(eta(2)-dithiolate) complexes [dithiolate = S2CNR2, DTCR (2a, R = Me; 2b, R = Et), (S2COPr)-Pr-i (3), and S2P((PrO)-Pr-i)(2) (4)]. Dichlorido substitution in 2 and 3 with DTCEt and (S2COPr)-Pr-i anions yielded Ru-IV derivatives containing bis(DTC) and mixed DTC-dithiocarbonate ligands. These are the first organoruthenium complexes of such ligands. The reaction of monophosphines with 2a resulted in monochlorido substitution, whereas the analogous reaction with 3 resulted in displacement of both chlorido ligands and reduction of the metal center to Ru-II. Reduction at Ru was also observed in the reaction of 2a with [CpCr(CO)(3)](2). Of these complexes, only 2 and 3 are air-stable in the solid state for an extended period. All of the complexes have been spectrally characterized, and selected compounds are also crystallographically characterized.