Vanadyl-phthalocyanine (VOPc) single crystals were prepared on KBr substrate by molecular beam epitaxy (MBE). Their maximum size is 1380.16 µm3. The morphology of the VOPc single crystal was investigated from the results of UV/VIS spectra and RHEED. They suggest that the VOPc single crystal may be grown with pseudomorphic layers. The growing process was expained by Volmer-Weber model. The third order nonlinear optical property of VOPc single crystal was measured with Maker fringe method. The value of the third order optical susceptibility (χ(3)) of VOPc single crystal was estimated to be about 10-9 esu from the result of Maker fringe.