In the 21st century, the optical computation is likely to be the basic technology for processing lots of information at high speed. The aim of the present research work is to develop optical logic gates or memory chips. For this purpose, we have examined the suitability of organic nonlinear optical dye material Vanadyl-phthalocyanine (VOPc). Large single crystals of this material have been fabricated by using Molecular Beam Epitaxy (MBE) technique. The epitaxial films were formed on the substrate under optimum operating conditions. However, the epitixial growth is observed only up to a limited thickness. Above this thickness, the films become non-epitaxial, which can be improved by annealing. The reformation of the epitaxial films has been confirmed. We have also reported the effects of the environment of high temperature on the multilayered tetra-tert-butyl-Vanadyl-phthalocyanine ((t-bu)4VOPc) films, formed by Langmuir-Blodgett (LB) method. The solvent used to dissolve ((t-bu)4VOPc) was 1,2-dichloroethane. The monolayer on the surface of the water was transferred to a glass substrate by the vertical dipping method. If the multilayered stack is too thick, the molecular arrangement of the film may get disturbed. The improvement in the molecular arrangement of the LB films was examined and confirmed by measuring it’s nonlinear optical susceptibility, using Maker Fringe Method. Monolayer formation on water surface depends on the surface pressure-area isotherm. If this monolayer formation is not perfect, multiplayer stacks cannot be formed. The molecular films were aligned almost perpendicular to the substrate, as estimated from the limiting molecular area of surface pressure-area isotherm. The molecular organization of the monolayer on the substrate and the molecular structure of the multilayered ((t-bu)4VOPc) films are discussed.