INTRODUCTIONCondensation of aldehydes with simple and higher molecular weight amines conducted in non-aqueous medium to extract hydrazides. Imines and substituted imines type Schiff's base ligands have been revealed to possess stronger coordination ability resulting in an emerging interest. It is well known that imines are not very stable compounds and are easy to hydrolyze. Hence, synthesis of free imine type Schiff"s base ligands in the metal free environment with high yield becomes more difficult due to their side polymerization reactions. One effective method to fix this problem involves an 'in situ' reaction. In other words, the metal ion acts as a templating agent, directing the condensation without polymerization.Research and review of literature show that the pH values play a vital role in determining the type of complexes formed during the course of the reaction. When the pH is between 5 and 6, the ligand does not ionize and mostly adopts the neutral (H2O)2] were assigned on the basis of hydrazine and metal analyses and further characterized by magnetic susceptibility measurements, UV-visible, infrared, 1 H and 13 C NMR and D2O exchange spectra, simultaneous TG-DTA analyses and X-ray powder diffraction techniques. The magnetic moments and UV-visible spectra indicate that these complexes are of high-spin octahedral geometry. The infrared spectra reveal the monodentate coordination of carboxylate ions and coordination of water molecules. The TG-DTA traces are in accordance with the formation of respective metal oxide as the end product after initial dehydration and further pyrolyses of the anhydrous complexes. The Xray powder diffraction patterns indicate the isomorphism among the series of complexes. In these complexes the metal ions are octahedrally surrounded by two bidentate hydrazoneglyoxylate ions and two water molecules. The isomorphism among the series of complexes has been exploited in the preparation of mixed metal complexes. The mixed metal complex when heated to 300 °C in a pre-heated silica crucible undergoes autocatalytic decomposition to yield respective metal cobaltite, MCo2O4 as the final residue. The formation of the mixed metal complexes and metal cobaltites are confirmed by their infrared spectra and X-ray powder diffraction patterns. TG-DTA of the complexes also supports the formation of metal cobaltites. The particle size and SEM analyses of simple oxides and mixed metal oxides were carried out for further application of these metal cobaltites as catalysts. The interaction of Zn(II) complex with calf thymus DNA was investigated by absorption spectra. The DNA binding affinity of Zn(II) complex is 2.60 × 10 4 M -1 which reveals the strong binding affinity.