The unidirectional crystal growth method has been employed for the bulk growth of semi-organic non-linear optical bisthiourea zinc chloride single crystal along a-axis with high solute-crystal conversion efficiency. Single crystal X-ray diffraction studies confirm the orthorhombic structure. Optical studies reveal very high transmission of the crystal along the growth axis. Dielectric study shows that the dielectric constant decreases with increase in frequency. Microhardness measurements along the growth axis enunciate the favorable hardness behavior. (C) 2009 Elsevier B.V. All rights reserved.