Bulk crystals of the charge-transfer complex, ethylenediamine-4-nitrophenolate monohydrate, were grown by slow solvent evaporation method from aqueous solution at room temperature. The X-ray diffraction measurements showed that the crystal belongs to centrosymmetric space group C2/c of monoclinic system. The functional groups in the complex were identified using FTIR, FTRaman and FTNMR analyses. The Z-scan measurements revealed the negative nonlinear refractive index of the crystal. The nonlinear absorption coefficient and third order nonlinear optical susceptibility calculated from the measurements were -3.5823 x 10(-3) cm/W and 2.3762 x 10(-6) esu respectively. The crystal was shown to be highly transparent above 366 nm by UV-vis spectroscopy and a yellow fluorescence was observed from PL spectrum. The TG-DTA and DSC analyses showed that the crystal is thermally stable up to 117.4 degrees C. The crystals were characterized by dielectric, etching and microhardness studies. (C) 2015 Elsevier Ltd. All rights reserved.