Cationic ligand N-methyl-4,4’-bipyridine (MQ) (Scheme 1) reacted respectively with metal halides and pseudohalides to form two organic-inorganic hybrid materials: [MQ][CuI2] (1), [Cu(MQ)(SCN)2] (2), which were characterized by single-crystal X-ray diffraction analyses, infrared spectra (IR), elemental analyses, powder X-ray diffraction (PXRD), and thermogravimetric (TG) analyses. The anion structure of compound 1 is binuclear and 2 is two-dimensional. Compounds 1- 2 show the better characteristic of degradating methylene blue (MB) in water under 500 W Xe vapor lamp irradiation.