Some bimetallic thiocyanate complexes exhibit excellent nonlinear optical properties. Single crystals of one such material Zinc Cadmium Thiocyanate ZnCd(SCN)4 abbreviated as ZCTC have been grown in Silica gel using gel technique by the process of diffusion. Colorless transparent crystals of size 12 mm × 2 mm × 1.3 mm have been obtained. Structural analysis has been carried out in powder form and for single crystal using X-ray diffractometer. Single crystal X-ray diffraction analysis reveals that the crystal lattice of ZCTC is tetragonal. From powder X-ray diffraction analysis the diffraction planes have been identified and unit cell parameters are determined. © 2007 Elsevier B.V. All rights reserved.