A novel single-component conductor derived from neutral radical gold bis(dithiolene) complexes is prepared based on the original reactivity of tBuN-substituted 1,3-thiazoline-2-thione heterocycle to give a tBuS-substituted thiazole ring. The corresponding 2-(tert-butylthio)-1,3-thiazole-4,5-dithiolate ligand (tBuS-tzdt) forms the d8 anionic complex [Au(tBuS-tzdt)2]−, easily oxidized through electrocrystallization into the neutral radical [Au(tBuS-tzdt)2]·. The effect of increasingly bulky R groups (R = Et, EtOH, tBu), in the series of such radical complexes [Au(RS-tzdt)2]·, is investigated, with a focus on their solid state organization, either into face-to-face dimers or into non-dimerized, uniform stacks.