Synthesis of zinc(II)/cadmium(II)/mercury(II) thiocyanate and azide complexes of a new bidentate Schiff-base ligand (L) with general formula of MLX2 (M = Zn(II), Cd(II), and Hg(II)) in ethanol solution at room temperature is reported. e ligand and metal complexes were characterized by using ultraviolet-visible (UV-visible), Fourier transform infrared (FT-IR), 1 H-and 13 C-NMR spectroscopy and physical characterization, CHN analysis, and molar conductivity.1 H-and 13 C-NMR spectra have been studied in DMSO-d6. e reasonable shis of FT-IR and NMR spectral signals of the complexes with respect to the free ligand con�rm well coordination of Schiff-base ligand and anions in an inner sphere coordination space. e conductivity measurements as well as spectral data indicated that the complexes are nonelectrolyte. eoretical optimization on the structure of ligand and its complexes was performed at the Becke's three-parameter hybrid functional (B3) with the nonlocal correlation of Lee-YangParr (LYP) level of theory with double-zeta valence (LANL2DZ) basis set using GAUSSIAN 03 suite of program, and then some theoretical structural parameters such as bond lengths, bond angles, and torsion angles were obtained. Finally, electrochemical behavior of ligand and its complexes was investigated. Cyclic voltammograms of metal complexes showed considerable changes with respect to free ligand.