A series of novel multidimensional transition metal-organic frameworks (MOFs), [Cu(Hbcpb)(2)](n), (1), [Co(bcpb)](n), (2), [Co(Hbcpb)(2)](1,4-bib)](n) (3) {[M(bcpb)(1-4-bimb)]center dot xH(2)O}n (M = Co (4), Cu (5), Ni (6), x = 1 for 5, 2 for 4 and 6), [Co(bcpb)(4,4'-bibp)](n) (7), {[Co(bcpb)(4.4'-bibp)]center dot 2H(2)O}(n) (8), and [Ni-2(bcpb)(2)(4,4'-bimp)(2)](n) (9), were synthesized under hydrothermal conditions in the presence of N-donor ancillary ligands [H(2)bcpb = 3,5-bis(3-carboxyphenyl)pyridine, 1,4-bib = 1,4-bis(1H-imidazol-4-yl)benzebe, 1,4-bimb = 1,4-bis(imidazol-1-ylemethyl)benzene, 4,4'-bibp = 4,4'-bis(imidazol-1-yl)biphenyl, 4,4'-bimp = 4,4'-bis(imidazol-1-ylmethyl)biphenyl]. Their structures have been determined by single-crystal X-ray diffraction analyses and further characterized by elementak analyses, IR sepectra, powder X-ray diffarction (PXRD), and thermogravimetric (TG) analyses. By adjusting the reaction pH, the H(2)bcpb ligand is partially deprotonated to give Hbcpb(-) form in 1 and 3, and completely deprotonated to afford the bcpb(2-) form in 2 and 4-9. Complex 1 exhibits a two-dimensional (2D) (3,6)-connected kgd topology