The imidazolium-2-dithiocarboxylate ligands IPr center dot CS2, Mes center dot CS2, and IDip center dot CS2 react with [AuCl(PPh3)] to yield [(Ph3P)Au(S2C center dot IPr))(+), [(Ph3P)Au(S2C center dot IMes)](+), and [(Ph3P)Au(S2C-IDip)](+), respectively. The compounds [(L)Au(S2C-IMes)](+) are prepared from the reaction of IMes center dot CS2 with [AuCl(L) (L = PMe3, PCy3, (CNBu)-Bu-t). The carbene-containing precursor [(IDip)AuCl] reacts with IPr center dot CS2 and IMes center dot CS2 to afford the complexes [(IDip)Au(S2C center dot IPr)](+) and [(IDip)Au(S2C center dot IMes)](+) with two carbene units, one bound to the metal center and the other to the dithiocarboxylate unit. Treatment of the diphosphine-gold complex [(dppm)(AuCl)(2)] with 1 equiv of IMes center dot CS2 yields [(dppm)Au-2(S2C center dot IMeS)](2+), while the reaction of [L-2(AuCl)(2)] (L-2 = dppb, dppf) with 2 equiv of IMes center dot CS2 results in [(L-2){Au (S2C center dot IMes)}(2)](2+). The homoleptic complexes [Au(S2C center dot IPr)(2)](2+), [Au(S2C center dot IMes)(2)](2+), and [Au(S2C center dot IDiP)(2)](2+) are obtained from the reaction of [AuCl(tht)] with 2 equiv of the appropriate imidazolium-2-dithiocarboxylate ligand. The compounds [(Ph3P)Au(S2C center dot NHC)](+) (NHC = IMes, IDip) and [(IDip)Au(S2C center dot NHC)](+) (NHC = IPr, IMes) are characterized crystallographically. The IMes center dot CS2 ligand is also used to prepare functionalized gold nanoparticles with diameters of 11.5 (+/-1.2) and 2.6 (+/-0.3) nm.