AbstractConducting organic metal chalcogenides (OMCs) have attracted considerable interest for their superior electrical properties and fascinating functions. However, the electronic structural and functional regulation of OMCs are typically limited to the combination of monometallic nodes and graphene-like ligands. Here, we report a family of bimetallic OMCs ([CuAg_x(C₆S₆)]_n, x = 4 or 2) synthesized via selective metal metathesis and oxidation transformation. Both OMCs have alternatively stacked one-dimensional (1D) copper-dithiolene chains and 2D Ag-S networks, which can synergistically serve as charge transport pathways, rendering these bimetallic materials highly conductive. The incorporation of heterometallic nodes turned nonmagnetic [Ag₅(C₆S₆)]_n into paramagnetic metallic [CuAg₄(C₆S₆)]_n, which exhibited a coherence-incoherence crossover in magnetic susceptibility measurements and an unusually large Sommerfeld coefficient, reminiscent of the characteristics of Kondo lattice. This work opens up an avenue for tailoring the electronic structures of OMCs and provides a platform for studying the dichotomy between electronic localization and itinerancy.