| Abstract | Four new mixed ligand nickel(II) complexes, viz., [Ni(Barb)2(H2O)4] 1, [Ni(Barb)2(en)2] 2, [Ni(Barb)2(pn)2] 3, and [Ni(Barb)2(BPA)(H2O)] 4 (Barb = 5,5 diethylbarbiturate, en = ethylenediamine, pn = propylenediamine, and BPA = bis(2 picolyl)amine) have been synthesized and characterized by means of elemental analysis, spectroscopic (FT-IR, Raman, and UV–Vis), and thermal analysis measurements. The spectral techniques suggest that all the nickel(II) complexes (1–4) exhibit octahedral geometry. The very low electrical conductance of the complexes supports their neutral nature. The monomeric nature of the complexes was assessed from their electronic spectra. X-ray diffraction studies were performed for the drug Barb-H and its nickel(II) complex 2. Complex 2 crystallizes in monoclinic space group P21/c with Z = 2. The barbital drug is N-coordinated and the en molecules act as bichelating ligands, leading to an NiN6 octahedral coordination. Molecules of complex 2 are connected via NAH_ _ _O hydrogen bonds, involving hydrogen atoms of both Barb and en ligands. The redox behavior of all complexes was investigated by cyclic voltammetry. Superoxide dismutase activity of these complexes has also been measured |