Nonlinear optical materials adopting optoelectronics elements are required to have a third-order nonlinear optical susceptibility of 10^(-9) order [esu]. However, the relationship between nonlinear optical characteristics and the morphology of the meal-phthalocyanine thin film prepared on alkali-halide substrate remains unclear. Therefore, the growing process of vanadyl-phthalocyanine (VOPc) thin films fabricated on alkali-halide substrate were investigated by UV/Vis spectra, AFM images, and the incident angle dependence of second harmonic (SH) and third harmonic (TH) intensities measured by Marker fringe. It is recognized that VOPc thin film prepared on KBr (100) is an island-like growth, on KCl (100) it is step-terrace growth.