The organic nonlinear optical crystal 4-chloroaniline was grown from methanol at room temperature by low temperature solution growth method. Powder X-ray diffraction was studied to confirm the grown crystal structure. The cutoff wavelength for the grown crystal was observed at 325 nm and the band gap energy of 3.814 eV was determined by recording the UV-Vis-NIR spectrum analysis. The presence of different functional groups of 4-chloroaniline were identified by FT-IR spectral analysis. The position of proton was found out by using 1H FT-NMR spectral analysis. The thermal stability of the crystal was carried out by TG-DTG analysis. The SHG efficiency for 4-chloroaniline was measured by Kurtz-Perry powder technique and the grown crystal is suitable for NLO application. © 2015 Scientific Publishers. All Rights Reserved.