Unprecedented helix-based MMOFs with a cylindrical channel constructed from a single, newly designed Na₂Pra₂biim [Na₂Pra₂biim = 1,1′-di(propionic acid)-2,2′-biimidazole disodium salt], [M(Pra₂biim)(H₂O)]_n·xnH₂O (M = Cd, Pb) have been presented, which are built from alternately arranged left- and right-handed helical M-biim tubes interconnected by the carboxyl arms of the ligand, and these findings reveal the promising potential of functionalized helical ligands in the construction of helix-based MMOFs from a single linker.