Vanadyl-phthalocyanine (VOPc) thin films were fabricated on KC1 (100) substrate by a molecular beam epitaxy. The morphologies of VOPc thin films fabricated under different preparing conditions were investigated by using Vis/ UV spectra, AFM images and the third order nonlinear optical properties measured with Maker fringe. The morphology of VOPc thin film on a KC1 substrate has three types. The first type has VOPc molecules tilted epitaxially on KC1 substrate, the second type has pseudomorphic VOPc layers on the epitaxial layer, and the third type is the bulk VOPc crystals deposited on the pseudomorphic layer. The third order nonlinear optical susceptibility estimated from a maximum third harmonic intensity of VOPc thin film measured by Maker fringe is about 10-9 esu. This is a practical value requested for the application to optical devices such as optical switching and memory.