Organic nonlinear optical material 4-chloroaniline (pCA) single crystal was grown by slow cooling method. The material solubility was determined by gravimetric analysis and the metastable zonewidth was measured at various temperatures. Induction period values were evaluated for different supersaturation ratio at different temperatures. The interfacial energies were calculated by experimentally determined induction period values. The energy results were theoretically compared with the experimental values derived from the solubility data. The nucleation parameters such as gibb’s free energy change, radius of the critical nuclei, number of molecules present in the nuclei and also nucleation rate were calculated. The unit cell parameters were determined by the X-ray diffraction analysis. pCA crystal transmission property was analyzed by UV-Vis-NIR spectrum. The various vibrational modes of different functional groups were identified and their wavenumbers were assigned from FT-Raman spectrum analysis. The nonlinear optical property of the grown crystal was measured by using Q-Switched Nd: YAG laser and the efficiency was compared to that of standard KDP. Copyright © VBRI Press.