The novel self-assembled zinc(5-acetamidoisophthalate) have been synthesized and characterized by elemental microanalysis, IR spectroscopy, thermogravimetric analysis and X-ray singlecrystal diffraction. 1, 2 and 3 are 1D coordination polymers that crystallize in monoclinic P2 1 , monoclinic P2 1 /m and triclinic P-1 systems, respectively, and are pseudo-polymorphic supramolecular isomers with 1 having a helical arrangement, and 2 and 3 exhibiting zig-zag type structures containing different guest molecules. Compound 4 crystallizes in the triclinic P-1 space group and is a 1D coordination polymer that exhibits fused 8-membered and 16-membered dimetallic rings. Compound 5 features a two-dimensional network type polymer with trimetallic cores. Compounds 1 -5 expand to 3D by means of H-bond interactions. These coordination polymers act as effective heterogeneous catalysts, under mild conditions, for the Knoevenagel condensation reaction of different aldehydes with an active methylene compound (malononitrile) and can be recycled without losing activity.