Bis thiourea cadmium acetate (BTCA) single crystals were grown at room temperature with different dopants by aqueous solution technique. The crystal system of the grown crystals with all the dopants was confirmed by powder X-ray diffraction study which confirms that there is no extra phase due to doping of L-alanine (LA), Mn(II) and glycine (Gly). It was further confirmed by FT-IR as well as FT Raman spectroscopy analysis. The effect of LA. Mn(II) and Gly doping on the crystalline perfection was assessed by high-resolution X-ray diffractometry (HRXRD) analysis which revealed that the grown crystals with Gly doping are more perfect in comparison of other dopants. The SHG efficiency was measured using the Kurtz powder technique and shows that the grown crystals with Gly doping are more efficient in comparison of other dopants which is in tune with crystalline perfection. The low values of dielectric constant and loss also revealed that the grown crystals are defect free. The hardness values were found to be increased by increasing the doping concentration. (C) 2012 Elsevier B.V. All rights reserved.