The new radical ligand 5,8-dimethyl-1,4-dioxonaphtho[2,3-][1,2,3]dithiazolyl () is reported. Two crystal polymorphs, and , differing in their pancake-bonded dimerization motif and S···O contact network, are identified. The self-assembly of Mn(II) metal ions with leads to the formation of that exhibits a Mn(II)-radical-Mn(II)-radical-Mn(II) linear arrangement of three Mn(hfac) units bridged by two radical ligands (hfac = 1,1,1,5,5,5-hexafluoroacetylacetonato-). Characterization by single-crystal X-ray diffraction of this Mn(II) complex packing structure reveals close noncovalent S···O contacts between the units in one dimension along the direction. The magnetic properties of the coordination complex are characterized by dc and ac susceptibility measurements on a microcrystalline solid. The magnetic data down to 4.8 K indicate the presence of effective ferromagnetic interactions (/ = +0.16 K) between the molecular = 13/2 units along the supramolecular chain involving noncovalent S···O contacts. Below 2.9 K, a non-zero out-of-phase component appears in the ac susceptibility, indicating the presence of a three-dimensional magnetic phase transition.
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