Zinc cadmium thiocyanate (ZnCd(SCN)(4), ZCTC) crystal is a promising nonlinear optical material as the source of blue-violet light by laser diode frequency-doubling. A series of experiments on the growth of ZCTC crystal are reported in this paper. A larger single crystal. with size 7 x 7 x 13 mm(3), was successfully obtained from the NH4Cl-NH4SCN-H2O mixed solvent by using the solvent-evaporation method. The problems in the growth of ZCTC single crystal are discussed and the key to growing large and transparent single ZCTC crystals is proposed.