The reaction of Ru-2(S2C3H6)(CO)(6) (1) with 2 equiv of Et4NCN yielded (Et4N)(2)[Ru-2(S2C3H6)(CN)(2)(CO)(4)], (Et4N)(2)[3], which was shown crystallographically to consist of a face-sharing bioctahedron with the cyanide ligands in the axial positions, trans to the Ru-Ru bond. Competition experiments showed that 1 underwent cyanation > 100x more rapidly than the analogous Fe-2(S2C3H6)(CO)(6). Furthermore, Ru-2(S2C3H6)(CO)(6) underwent dicyanation faster than [Ru-2(S2C3H6)(CN)(CO)(5)](-), implicating a highly electrophilic intermediate [Ru-2(S2C3H6)(mu-CO)(CN)(CO)(5)](-) Ru-2(S2C3H6)-(CO)(6) (1) is noticeably more basic than the diiron compound, as demonstrated by the generation of [Ru-2(S2C3H6)-(mu-H)(CO)(6)](+), [1H](+). In contrast to 1, the complex [1H](+) is unstable in MeCN solution and converts to [Ru-2(S2C3H6)(mu-H)(CO)(5)(MeCN)](+). (Et4N)(2)[3] was shown to protonate with HOAc (pK(a) = 22.3, MeCN) and, slowly, with MeOH and H2O. Dicyanide [3](2-) is stable toward excess acid, unlike the diiron complex; it slowly forms the coordination polymer [Ru-2(S2C3H6)(mu-H)(CN)(CNH)(CO)(4)](n), which can be deprotonated with Et3N to regenerate [H3](-). Electrochemical experiments demonstrate that [3H](-) catalyzes proton reduction at -1.8 V vs Ag/AgCl. In contrast to [3](2-), the CO ligands in [3H](-) undergo displacement. For example, PMe3 and [3H](-) react to produce [Ru-2(S2C3H6)(mu-H)(CN)(2)(CO)(3)(PMe3)](-). Oxidation of (Et4N)(2)[3] with 1 equiv Of Cp2Fe+ gave a mixture of [Ru-2(S2C3H6)(mu-CO)(CN)(3)(CO)(3)](-) and [Ru-2(S2C3H6)(CN)(CO)(5)](-), via a proposed [Ru-2](2)(mu-CN) intermediate. Overall, the ruthenium analogues of the diiron dithiolates exhibit reactivity highly reminiscent of the diiron species, but the products are more robust and the catalytic properties appear to be less promising.