By introducing an amino substituent group on the dicarboxylate ligand, a porous doubly pillared-layer framework [Co 2(abdc) 2(bpy) 2]•8DMF (2; abdc = 2-amino-1,4-benzene dicarboxylate, bpy = 4,4′-bipyridine) has been obtained, which represents a shape/size modulation of the layer apertures to control over 2-fold interpenetration arising from the nonporous structure of [Co 2(bdc) 2(bpy) 2] (1; bdc = 1,4-benzene dicarboxylate). The bulk-phase purity, framework robustness and permanent porosity of 2 have been confirmed by powder X-ray diffraction, thermogravimetric analys...