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 d
14 and d
25 with the simultaneously applied dc- and UV-laser fields were investigated and discussed.