One compound with N-（4-pyridylmethyl）imidazole liand, [Co（pyim）2（N3）2]n 1 （pyim = N-（4-pyridylmethyl）imidazolv）, was synthesized and structurally characterized. Compound 1 crystallizes in triclinic, space group P21/c with a = 8.090（3）, b = 16.109（3）, c = 8.590（3）, β = 117.800（12）°, V= 990.3（5） A3, Z= 2, Mr = 46137, Dc = 1.547 g/cm3, F（000） = 474, μ= 0.901 mml, the final R = 0.0381 and wR = 0.0950 for 1581 observed reflections with I〉 2o（I）. In this compound, the unique Co（II） resides at a crystallographic inversion center and exhibits an octahedral coordination geometry. The adjacent Co（II） ions are connected by the pyim ligands to form a 2D layer structure. The layers are stacked in an ABAB mode and reinforced by the weak interlayer C-H.-.N hydrogen bonds and π-π stacking to give a 3D architecture. The thermal properly and electrochemical property of compound 1 have also been studied.
