Three-component reactions involving Ni(II) ions and dicarboxylate and bipyridyl ligands under hydrothermal conditions produce two novel metal–organic coordination polymers formulated empirically as [Ni(PDA)(BPE)] (1) and [Ni 2 (PDA) 2 (BPP)(H 2 O)]·2.5H 2 O (2), where PDA=1,4-phenylenediacetate, BPE=1,2-bis(4-pyridyl)ethane, and BPP=1,3-bis(4-pyridyl)propane. Both compounds possess 2D or 3D metal–organic frameworks (MOFs) that are assembled on dinickel-carboxylate secondary building units. Compound 1 has a condensed 3D MOF, whereas 2 contains void between 2D MOFs where guest water molecules reside. Both compounds demonstrate antiferromagnetic coupling between Ni(II) ions.