In the last few decades, researchers have aimed at finding high quality materials from the complex crystal family. Some of the bimetallic complexes of thiocyanate crystallize into noncentrosymmetric space group which confirms the second harmonic generation. In the AB(SCN)4 molecules, metal ions can bind to SCN− ion through either sulfur or nitrogen [1] and [2]. When compared with the inorganic materials, the applications of organic nonlinear optical crystals are limited because of their poor chemical stability and poor phase matching. The main advantage of choosing metal complexes is that they offer a large variety of structures, higher environmental stability and a much greater diversity of tunable opto electronic properties [3] and [4]. Some of the doped crystals of the bimetallic thiocyanate complexes are also found to exhibit good nonlinear optical properties [5]. In the present work an attempt has been made by substituting certain amount of Ni2+ by Cu2+ in the already reported crystal nickel mercury thiocyanate (NMTC) [6]. The characterization of the grown crystal was compared with the pure NMTC crystal.