N-aryl heterocycles have attracted increasing attention due to their wide applicability in biochemical,biological,medicinal and material sciences.1 The most straightforward routes for synthesis of N-arylazole derivatives involve copper-mediated Uilmann-type coupling2 and Pd-catalyzed Buchwald-Hartwig reaction of nitrogen-containing heterocycles with aryl halides.3 These reactions require expensive catalysts,or hard reaction conditions (such as high reaction temperature) and produce large amount of harmful wastes.Since 1998,the Chan-Lam coupling reaction4 has emerged as a highly efficient and valuable alternative to traditional methods for the construction of C-N bond due to the wide variety of commercially available boronic acids and the mildness of the reaction conditions.5 In this paper,we have designed and prepared a set of N,N-bidentate coordination ligands attached 1-methyl-pyridinium group (1-methyl-((pyridinyl)pyrazolyl)pyridin-1-ium iodide ([pypzpym]Ⅰ)),which were obtained by reactions of 3,2-pypzpy,4,2-pypzpy,2,3-pypzpy or 2,4-pypzpy with excess MeI in refluxing THF.Reactions of CuI with these ligands afforded five anionic[CuxIy]-based coordination complexes[Cul2(3,2-pypzpym)](1),[Cu4I6]n[(3,2-pypzpym)2n](2),[Cu4I6(4,2-pypzpym)2](3),[CuI2(2,3-pypzpym)](4) and[(CuI2)(2,4-pypzpym)](5).Compared with that of CuI,complexes 1-5 displayed greatly enhanced catalytic activities toward the coupling of imidazole with arylboronic acid in H2O/MeCN (v/v =2∶1).