The assembly of Cu(CH3COO)2·H2O and pyridine-4,5-imidazoledicarboxylic acid (H3PyImDC) under solvothermal conditions in the presence of different organic templates yielded two three-dimensional chiral frameworks, (C3H10N 2)(C3H7NO)0.5- (H2O) 2[CuIIC10H5O4N 3] (1) and |(C4H9NO)0.5(H 2O)8[CuII2CuI(C 10H5O4N3)2(C 10H6O4N3)] (2). Both of the compounds crystallized in the cubic, P4332 space group and possessed open helical channels in the frameworks. To the best of our knowledge, compounds 1 and 2 present the first synthesized MOFs with a bmn and lcy-a net. Further characterization of the two compounds has been performed, including X-ray powder diffraction, inductively coupled plasma analysis, CHN, IR spectra, fluorescence spectra, X-ray photoelectron spectroscopy spectrum and thermogravimetric- differential thermal analysis.