The reaction of Ru(Et(2)dtc)(2)(DMSO) (Et(2)dtc = N,N-diethyldithiocarbamate; DMSO = dimethyl sulfoxide) with t-BuNC gave trans-Ru(Et(2)dtc)(2)(CN-t-Bu)(2), 1. Complex 1 crystallizes in the monoclinic space group P2(1)/n with 9.753(2) Angstrom, b = 11.583(2) Angstrom, c = 12.974(2) Angstrom, and beta = 91.8(2)degrees for Z = 2. The crystal structure of 1 shows the trans disposition of the two isocyanides; the mean Ru-S and Ru-C distances are 2.409 and 1.477(2) Angstrom, respectively. Treatment of [Ru(diene)Cl-2](n) with Na(Et(2)dtc) afforded Ru(Et(2)dtc)(2)(diene) (diene = bicyclo[2.2.1]-hepta-2,5-diene (NBD), 2, 1,5-cyclooctadiene (COD), 3). Complex 2 crystallizes in the triclinic space group P (1) over bar with a 7.316(1) Angstrom, b = 10.346(1) Angstrom, c = 15.123(2) Angstrom, alpha = 103.69(2)degrees, beta = 93.54(2)degrees, and gamma = 100.61(2)degrees for Z = 2. The mean Ru-S and Ru-C distances in 2 are 2.416 and 2.137 Angstrom, respectively. The reaction of cis-Ru(Et(2)dtc)(2)(CO)(2) with iodine gave the 2:1 molecular iodine complex cis-Ru(Et(2)dtc)(2)(CO)(2).1/2 I-2 4, which crystallizes in the monoclinic space group P2(1)/c with a = 7.347(2), b = 22.227(2) Angstrom, c = 12.891(2) Angstrom, and beta =95.98 (2)degrees for Z = 4. The mean Ru-S and Bu-C and the I-l distances in complex 4 are 2.427, 1.903, and 2.745(1) Angstrom, respectively. Treatment of Ru(Et(2)dtc)(2)(DMSO)(2) with I-2 gave the linear Ru(II)-Ru(III)-Ru(III) trimer [Ru-3(Et(2)dtc)(6)(DMSO)(2)](I-3)(2), 5, which crystallizes in the triclinic space group P (1) over bar with a = 14.125(3) Angstrom, b = 20.829(6) Angstrom, c = 13.658(3) Angstrom, alpha = 97.57(2)degrees, beta = 110.01(2)degrees, and gamma = 71.25(2)degrees for Z = 2. The structure of complex 6 can be viewed as consisting of a {Ru-2(III)(Et(2)dtC)(4)}(2+) Core and a (Ru-II(Et(2)dtc)2(DMSO)(2)} moiety, which are linked together via the two dithiocarbamate sulfurs of the latter. While the two Ru(III) centers are connected by a Ru-Ru single bond (Ru-Ru = 2.826(2) Angstrom, there is no direct interaction between the Ru(III) and Ru(II) centers. Oxidation of Ru(Et(2)dtc)(2)L-2 (L = PPh3, t-BuNC) by I-2 gave the respective [Ru(Et(2)dtc)(2)L-2](+) cations. The reaction of cis-Ru(Et(2)dtc)(2)(PPh3)(2) with excess tosyl azide gave the diamagnetic Ru(IV) tetrazene complex Ru(Et(2)dtc)(2)(Ts2N4), 7, Complex 7 crystallizes in the triclinic space group P (1) over bar with a 10.380(1) Angstrom, b = 11.322-(1) Angstrom, c = 15.310(1) Angstrom, alpha = 106.54(2)degrees, beta = 106.87(2)degrees, and gamma = 92.63(2)degrees for Z = 2. The Ru-S and Ru-N-alpha distances in 7 are 2.385 and 1.98 Angstrom, respectively. The formal potentials of the Ru dithiocarbamate complexes were determined by cyclic voltammetry.