Single crystals of cadmium mercury thiocyanate glycol monomethyl ether (CMTG) were grown from a mixed solvent of glycol monomethyl ether (GME):water (1:1) by slow evaporation method. The crystal structure and morphology were confirmed by single crystal X-ray diffraction analysis. Presence of functional groups and the coordination of glycol monomethyl ether (GME) and thiocyanate (SCN(-)) in the CMTG compound were confirmed by FT-IR analysis. Optical transparency of the grown crystal was studied by UV-Vis spectroscopy. Thermal stability and decomposition process were studied by means of TGA and DTA analysis. Dielectric measurement on CMTG single crystal was carried out for various frequency and temperatures. The surface studies by scanning electron microscopy reveals the formation of layer growth pattern indicative of 2D nucleation mechanism. From the second harmonic Output power measurement by Kurtz powder method, it is observed that CMTG is a potential material for nonlinear optical applications among the bimetallic thiocyanate adducts series. (C) 2009 Elsevier B.V. All rights reserved.