The hydrothermal reaction of fumaric acid, benzylamine, and metal salts yielded MRrac-N-benzyl-Asp) (H2O)] (M = Co, Ni), 1 and 2, and NiRrac-N-benzyl-Asp)(H2O)(3)]center dot H2O 3. Under mild hydrothermal conditions, Michael addition of benzylamine to fumaric acid led to the formation of a racemic mixture of N-benzyl aspartic acid enantiomers. The noncentrosymmetric structures of 1 and 2 consist of one-dimensional polymeric chains in which metal cations are bridged by D- and L-N-benzyl aspartate anions alternating along the chain. The centrosymmetric structure of 3 is composed of discrete Ni[(rac-N-benzyl-Asp)(H2O)(3)] units that are connected by hydrogen bonds into layers. The single layers are homochiral but are hydrogen bonded to similar homochiral layers that contain the N-benzyl aspartate with the opposite handedness. Compounds 1 and 2 showed second harmonic generation (SHG), and their magnetic and thermodynamic properties are described.