A new inorganic-organic hybrid material, [EtdiPy][Co(NCS) 4 ] (1) ([EtdiPy] 2þ ¼ 1,1 0 -ethylene-2,2 0 -dipyridinium), was synthesized and characterized by elemental analysis, IR spectrum, UV-Vis spectrum, ESI-MS, and single-crystal X-ray diffraction. Compound 1 is monoclinic, (3) , V ¼ 4075.1(16) Å 3 , D c ¼ 1.550 g cm À3 , Z ¼ 8, F(000) ¼ 1928, and R 1 ¼ 0.0435. The C-HÁ Á ÁS hydrogen bond, short SÁ Á ÁC, SÁ Á ÁN interactions, pÁ Á Á, and Á Á Á interactions observed in the solid state of 1 give a 3-D structure. Magnetic measurements from 2 to 300 K have shown weak antiferromagnetic exchange with ¼ À0.892 K in 1.