Stable monolayers of the Schiff base of O-Vaniline have been formed at the air/water interface and on a subphase containing Cu2+, Ni2+ and Zn2+ ions. Polarized UV-Visible spectra of the Langmuir-Blodgett (LB) films of the pure Schiff base and those of the metal complexes on solid substrates have been studied. The LB films indicate that the aromatic rings in the polar plane are oriented slightly out of plane to the solid substrate and the orientation remains nearly the same for the ligand and for the complexes. Low angle XRD shows that the copper complex and the ligand stack into multimeric structures as the monolayer is compressed on the water surface.