Reaction of H3TDA with PrIII/NdIII salts resulted in two coordination polymers, [Ln(H2O)4(HTDA)(H2TDA)]·H2O (Ln = Pr(1) and Nd(2), H3TDA = 1H-[1,2,3]-triazole-4,5-dicarboxylic acid), crystallizing in the monoclinic P21/c space group with a one-dimensional zigzag chain structure. The number of ligands and water molecules coordinated to the LnIII ions can be reduced by a hydrothermal method and the products transformed into {[Ln(TDA)(H2O)]·2.5H2O}n (Ln = Pr(3) and Nd(4)), crystallizing in the trigonal P3121 space group with a three-dimensional chiral framework structure. The compounds were characterized by elemental analysis, IR, PXRD, circular dichroism spectra and single crystal X-ray diffraction. The variable temperature magnetic susceptibility studies indicated that there are antiferromagnetic interactions between the LnIII ions in 1–4. Gas sorption and separation were studied as well.