This paper reports the synthesis, structure solution, and magnetic characterization of four new DIMMAL-containing compounds (H(2)DIMMAL = 2-di1H-2-imidazolylmethylmalonic acid), H(2)DIMMAL center dot H2O (1), Na-2(DIMMAL)-5H(2)O (2), [Cu(HDIMMAL)(2)] (3), and [Cu-2(DIMMAL)(2)(H2O)(2)]center dot 2H(2)O (4). Compound 1, containing two carboxylates and two protonated imidazole rings, adopts the dizwitterion configuration. These monohydrate MBBs pack together into a 3D array driven, as in the other three cases herein reported, by a combination of multiple-path H-bonds and aromatic-aromatic interactions. Compound 2 consists of centrosymmetric Na+ tetramers in which four NaO6 distorted octahedra are interconnected by carboxylate and water bridges. Compound 3 consists of mononuclear [Cu(HDIMMAL)(2)] units in which HDIMMAL(-) acts as a tridentate ligand through two imidazole N atoms and the deprotonated O from a carboxylate. Compound 4 consists of centrosymmetric cyclic dinuclear [Cu-2(DIMMAL)(2)(H2O)(2)]center dot 2H(2)O units involving propionate-arm bridges. The building-block units described above, in each case, are interconnected into 3D networks by multiple H-bonding paths and aromatic-aromatic interactions. The EPR spectra are indicative of an essentially d(x2-y2) ground state for the copper(II) ions in 3 and 4 (CuN4O2 and CuN2O2O' chromophores, respectively). Magnetic susceptibility measurements in the range of 1.8-200 K for compound 4 show weak antiferromagnetic exchange between the copper(II) ions (2J = -1.6(1) cm(-1)). The effectiveness of the propionate-arm bridges, involving C-C a bonds, in propagating magnetic exchange between the copper(II) ions is discussed.