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This contribution describes metal-organic frameworks based on cadmium-clusters that are capable of generating double-pillared architectures. A brief overview of the literature concerning such systems is presented together with the description of three new coordination polymers, [{[Cd2(trans-1,2-a,a-chdc)(trans-1,2-e,e-chdcH)2(4,4′-bpy)2]·8H2O}n] (1), [{Cd2(trans-1,4-e,e-chdc)(trans-1,4-a,a-chdc)(4,4′-bpe)2}n] (2) and[{[Cd2(cis,cis-1,3,5-chtc)(HCO2)(H2O)(4,4′-bpy)2]·DMF·4H2O}n] (3) [1,2-chdc = 1,2-cyclohexanedicarboxylate, 1,4-chdc = 1,4-cyclohexanedicarboxylate, 1,3,5-chtc = 1,3,5-cyclohexanetricarboxylate, 4,4′-bpy = 4,4′-bipyridine and 4,4′-bpe = (E)-1,2-bis(4-pyridyl)ethylene]. Compound 1 has a double-pillared two-dimensional layer structure, while compounds 2 and 3 are double-pillared three-dimensional frameworks. All materials have been characterized by elemental analysis, IR spectroscopy, single-crystal X-ray diffraction and thermogravimetric analysis. The robustness of the open-frameworks found for compounds 1 and 3 has been examined by X-ray powder diffraction of dried samples, which showed that the crystal structure of the 2D coordination polymer 1 collapses whereas the 3D architecture of compound 3 remains intact. (© Wiley-VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2008)