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The title complex was a Mott insulator, in which the head-to-head type dimer of newly synthesized donor molecule, 2-(thiapyran-4-ylidene)-4,5-ethylenedioxy-1,3-dithiole (TP-EDOT) accommodated a localized spin. Although the localized spins were arranged in three-dimensional (3D) framework, the interaction between them was interpreted as a two-dimensional (2D) spin system. The ability of TP-EDOT to exhibit intermolecular interactions along the molecular longitudinal axis allowed to form a head-to-head dimer, which provided an elongated space to reserve a localized spin. The anisotropy of this dimer was regarded to be the origin of the novel 2D spin structure formed in the 3D lattice. [ABSTRACT FROM AUTHOR]