Two novel metal-organic frameworks with different structures were obtained by reactions of Pbl(2) with N,N'-bis(3-pyridylmethyl)-1,4-biphenylenedimethyleneimine (L) under different M/L ratios. When the M/L ratio is 1:1, L bridges [Pbl(2)](n) chains to form a layered organic-inorganic hybrid compound with the empirical formula [Pb(L)I-2] (1). When changing the M/L ratio to 2:1, L bridges the double chains [Pb-2(L)I-4](n) to form networks [Pb-2(L)I-4] (2), which are further linked by C-(HI)-I-... hydrogen bonds to give a 3D structure.