In this paper, we report the synthesis, growth and characterization of a new organic NLO single crystal of NMPMN (N'-[(Z)-(4-methylphenyl)methylidene]-4-nitrobenzohydrazide), for the first time. The single crystal was grown by slow evaporation method at room temperature. The cell dimensions obtained by single crystal XRD studies reveal that the crystal belongs to triclinic system. It was characterized by different techniques like powder XRD, UV, FTIR, TGA and DSC. The Knoop microhardness test was carried out to measure the mechanical strength of the crystal. Its refractive index was determined by the Brewster's angle method. The laser damage threshold studies have been carried out for the crystal using a Q-switched Nd:YAG laser of ns pulses at a wavelength of 532 nm. The Kurtz Powder Second Harmonic Generation revealed that the SHG efficiency of the grown crystal is about 50% that of KDP and is found to be phase matchable. The intermolecular O-H center dot center dot center dot O, O-H center dot center dot center dot N and C-H center dot center dot center dot O hydrogen bonds and a pi-pi stacking interaction between the nitrobenzene and tolyl rings helps to create a delicate balance between the molecular and supramolecular charge transfer processes by creating a noncentrosymmetric structure. (C) 2010 Elsevier B.V. All rights reserved.