Single crystals of pure and potassium iodide (Kl)-doped Zinc Tris-thiourea Sulphate (ZTS) were grown from aqueous solutions by slow evaporation technique. The grown crystals have been subjected to single crystal X-ray diffraction to determine the unit cell dimensions. The grown crystals were also characterized by recording the powder X-ray diffraction patterns and by identifying the diffracting planes. The Fourier Transform Infrared (FT-IR) spectra have been recorded in the range 400-4500cm(-1). Second harmonic generation (SHG) for the materials of this work was confirmed using Nd:YAG laser. The UV-visible spectra show that the grown crystals have wide optical transparency in the entire visible region. The Thermogravimetric/Differential Thermal Analyses (TG/DTA) thermograms reveal that the materials have good thermal stability. Atomic absorption study reveals the presence of potassium in the doped f crystals. The electrical measurements were made in the temperature range 40-130 degrees C along c-direction of the grown crystals. The dielectric studies show that there may be a ferroelectric transition at 50 C for both pure and KI-doped ZTS crystals. DC conductivity for both the samples is found to be increasing with increase in temperature. Activation energy values were also determined for both AC and DC conduction processes in the samples. (C) 2008 Elsevier B.V. All rights reserved.