An amino-functionalized terphenyl-tetracarboxylic acid, 2′-amino-[1,1′:4′,1″-terphenyl]-3,3″,5,5″-tetracarboxylic acid (H 4 tpta), was used as an adaptable linker to synthesize, under hydrothermal conditions, eight coordination polymers (CPs). The obtained products were formulated as [Co(μ 6 -H, wherein 2,2′-bipyridine (2,2′-bipy), 4,4′bipyridine (4,4′-bipy), 1,10-phenanthroline (phen), or 2,2′-biimidazole (H 2 biim) are present as additional stabilizing ligands. The structural types of 1−8 vary from onedimensional (1D) (2, 5) and two-dimensional (2D) (3, 4, 6) CPs to three-dimensional (3D) metal−organic frameworks (MOFs) (1, 7, and 8) with a diversity of topologies. The products 1−8 were investigated as catalysts in the Knoevenagel condensation involving aldehydes and active methylene derivatives (malononitrile, ethyl cyanoacetate, or tertbutyl cyanoacetate), leading to high condensation product yields (up to 99%) under optimized conditions. Various reaction conditions, substrate scope, and catalyst recycling were investigated. This work broadens the application of H 4 tpta as a versatile tetracarboxylate linker for the generation of diverse CPs/MOFs.