When Ni(NO3) 2•6H2O and N,4,5, are reacted, a one-dimensional coordination polymer (1) is formed. However, reaction with either terephthalic acid (2) or 2,6-naphthalenedicarboxylic acid (3) affords two-dimensional, pillared metal-organic frameworks. 2 and 3 containing rectangular voids of different dimensions which are dictated by the carboxylate ligand and the arrangement of the [M(k 2 -O2NO)]2(µ 2 -O2CR)2] secondary building unit (SBU) that forms the nodes of the framework. The role of SBU geometry, intermolecular face-to-face π-π and lone pair-π interactions involving the DPNDI ligands are discussed.