Organic nonlinear optical crystals of 2-hydroxy-3-methoxy-N-(2-chloro-benzyl)-benzaldehyde-imine has been successfully grown by low temperature solution growth technique. The grown crystals were characterized by single crystal XRD, FTIR, TGA/DTA and UV-vis-NIR techniques. Nonlinear optical property of the crystal was studied by Kurtz powder technique using Nd: YAG laser and the crystal exhibits second harmonic generation property. (c) 2009 Elsevier B.V. All rights reserved.