Using ethanol as a solvent p-aminoazobenzene (p-AAZB), an organic nonlinear optical crystal having good optical quality was grown by slow evaporation solution technique. Structural and optical properties were studied by applying XRD and UV-Vis spectroscopy. The measurement of the second harmonic generation was performed using the fundamental Nd:YAG 10 ns laser beam with wavelength 1.064 μm. Dependence of the second order susceptibilities for the two principal second order susceptibility tensor components d14 and d25 with the simultaneously applied dc- and UV-laser fields were investigated and discussed.