In the present contribution, some novel Cu(II) complexes were synthesized from tri- and tetradentate imine ligands. All the prepared compounds were elucidated by different physicochemical methods. Density Functional Theory calculations were carried out to explain the equilibrium geometry of the bsisnph and npisnph ligands and their Cu(II) complexes. Interaction of the synthesized ligands with Cu(II) affords nano-sized particles via TEM. The catalytic potentials of the prepared complexes has been tested within the oxidation of benzyl alcohol using an environmental friendly terminal oxidant, i.e. H2O2. The effect of various parameters, e.g. solvents, temperature and amount of catalyst was investigated. A mechanistic pathway of the catalytic oxidation was tentatively described and discussed. [GRAPHICS]