a b s t r a c tDescribed are the synthesis and characterization of two, potentially tetradentate, N 2 S 2 Schiff-base ligands, containing a disulfide bond, N, and L 2 and the complexes 1 and 2 have been characterized spectroscopically, and the crystal and molecular structures of the two complexes have been determined by single crystal X-ray diffraction. The coordination geometry around Zn(II) centers in both complexes is a distorted tetrahedron. In addition, DFT calculations (B3LYP/LANL2DZ/6-311++G(d,p)) support the structure of 1. Cyclic voltammetric studies demonstrate that Zn(II) shifts the reduction potential of the disulfide ligands L 1 and L 2 to less negative values thus making them more susceptible to reductive cleavage of the disulfide bond. The results of semi-empirical PM6 calculations offer key insight into the nature of the transition state for this reaction.