Two Ni(II) coordination polymers, namely {[Ni(L1)(2,6-ndc)(0.5)(H2O)(2)]center dot 0.5(2,6-ndc)center dot 2H(2)O} (n) (1) and [Ni(L2)(1,4-ndc)(H2O)] (n) (2) (L1 = 1,3-bis(5,6-dimethylbenzimidazol-1-yl)-2-propanol, L2 = 1,3-bis(5,6-dimethylbenzimidazol-1-ylmethyl)benzene, 2,6-H(2)ndc = 2,6-naphthalenedicarboxylic acid and 1,4-H(2)ndc = 1,4-naphthalenedicarboxylic acid) have been synthesized under hydrothermal conditions and structurally characterized by elemental analyses, thermogravimetric analysis, IR spectra, and single crystal X-ray diffraction. CP-1 presents a 1D zigzag chain, and CP-2 features a 1D tube-like chain. Both one-dimensional coordination polymers are further extended into 3D and 2D supramolecular framework via classical O-H center dot center dot center dot O hydrogen bondings, respectively. Moreover, the catalytic properties of the two complexes for the degradation of Methyl orange in a Fenton-like reaction are discussed. [GRAPHICS] .