Three novel complexes all with multidimensional frameworks containing Group 12 metals linked by pyrazine and thiocyanate ligands have been prepared. The complexes reported here are [Zn(NCS)2(Pyz)2]n (1), [Cd(NCS)2(Pyz)]n (2), [Hg(NCS)2(Pyz)]n (3) and were characterized by elemental analysis, mid- and far-range FT-IR, and 1H and 13C NMR spectroscopy. Fluorescence properties have been investigated. Structures of all three compounds have been confirmed by single crystal X-ray diffraction. The 2-D zinc structure consists of a distorted N6 octahedron comprised of bridging pyrazine moieties and pendant thiocyanate ligands. Both Cd and Hg coordination polymers consist of an N4S2 distorted octahedral kernel with pyrazine molecules bridging along the y-axis and the double-chain thiocyanate bridging in the x and z directions creating a 2-D ladder type structure. Soft-Soft non-covalent interactions between the thiocyanate ions on neighboring molecules extend the Zn and Cd structures to three dimensions. Compounds (1) and (2) are found to be non-centrosymmetric.