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A novel copper(II) thiocyanate complex [Cu(im)2(NCS)2] 1 (im=imidazole) has been prepared and characterized by spectroscopic analysis and crystallographic method. This supramolecular compound exhibits a three-dimensional solid state structure constituted by N–H⋯S hydrogen bonds and π–π stacking interactions. The compound in DMF solutions has a very strong third-order non-linear optical (NLO) behavior with absorption coefficient and refractive index α2=1.18×10−11 m w−1, n2=−9.00×10−16 m2 w−1, respectively, and third-order NLO susceptibility χ(3) of 7.00×10−10 esu. [Copyright &y& Elsevier]