A promising strategy for new electrically conductive coordination polymers is the combination of d(10) metal ions, which tolerate short metal center dot center dot center dot metal distances, with dithiolene linkers, known for their "non-innocent" redox behavior. This study explores the coordination chemistry of 2,3-pyrazinedithiol (H(2)pdt) toward Cu+ and Ag+ ions, highlighting similarities and differences. The synthetic approach, starting with the fully protonated ligand, allowed the isolation of a homoleptic bis(dithiolene) complex with formal CuI atoms, [Cu(H(2)pdt)(2)]Cl (1). This complex was further transformed to a 1D coordination polymer with short metal center dot center dot center dot metal distances, 1D[Cu(Hpdt)] (2Cu). The larger Ag+ ion directly built up a very similar coordination polymer, 1D[Ag(Hpdt)] (2Ag), without any appearance of an intermediate metal complex. The coordination polymer 1D[Cu(H(2)pdt)I] (4), like complex 1, bears fully protonated H(2)pdt ligands in their dithione form. Upon heating, both compounds underwent auto-oxidation coupled with a dehydrogenation of the ligand to form the open-shell neutral copper(II) complex [Cu(Hpdt)(2)] (3) and the coordination polymer 1D[Cu2I2(H(2)pdt)(Hpdt)] (5), respectively. For all presented compounds, crystal structures are discussed in-depth. Furthermore, properties of 1, 3, and those of the three 1D coordination polymers, 2Ag, 2Cu, and 4, were investigated by UV-vis-NIR spectroscopy, cyclic voltammetry, and variable-temperature magnetic susceptibility, and direct current (dc)-conductivity measurements. The experimental results are compared and discussed with the aid of DFT simulations.