A hydrazone oxime (H2L) has been prepared in EtOH by reacting 2-hydrazine hydrate (2) with 2,3-butanedione monoxime (1). Homodinuclear copper(II), nickel(II), homotetranuclear copper(II), and heterotetranuclear copper(II)-nickel(II) complexes of H2L have been prepared. The metal complexes have been characterized by elemental analyses, magnetic moments, infrared (IR), ultraviolet-visible (UV-vis), and mass and thermal analyses studies. The dinuclear copper(II) and nickel(II) complexes of H2L were found to have a 1: 1 metal: ligand ratio. In addition, total energy and heat formation for ligands (H2L and DHyLH(2)) by semiempirical PM3 calculations have shown that H2L is more stable than DHyLH(2).