One compound with N-(4-pyridylmethyl)imidazole liand, [Co(pyim)(2)(N-3)(2)](n) 1 (pyim = N-(4-pyridylmethyl)imidazole), was synthesized and structurally characterized. Compound 1 crystallizes in triclinic, space group P2(1)/c with a = 8.090(3), b = 16.109(3), c = 8.590(3), beta = 117.800(12)degrees, V = 990.3(5) angstrom(3), Z = 2, M-r = 461.37, D-c = 1.547 g/cm(3), F(000) = 474, mu = 0.901 mm(-1), the final R = 0.0381 and wR = 0.0950 for 1581 observed reflections with I > 2 sigma(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 center dot center dot center dot N hydrogen bonds and pi-pi stacking to give a 3D architecture. The thermal property and electrochemical property of compound 1 have also been studied.