Single crystals Of DL-malic acid-doped ammonium dihydrogen phosphate have been grown using slow evaporation method and also by Sankaranarayanan-Ramasamy (SR) method with the vision to improve the properties of the ADP crystals. The characterization of grown crystals was made by single-crystal X-ray diffraction, powder X-ray diffraction, UV-vis. spectroscopy, Fourier transform infrared spectroscopy (FTIR), differential thermal analysis (DTA), Vicker's microhardness, dielectric measurements, high-resolution X-ray diffraction (HRXRD) and second-harmonic studies. Structural difference between pure and doped crystal has been studied by XRD analysis. Functional groups were identified by FTIR spectroscopy. The grown crystals were found to be transparent in the entire visible region. Decomposition temperatures of the grown crystals were measured by DTA. Vicker's hardness study carried out on (0 0 1) face at room temperature shows increased hardness of the doped crystals and SR-method-grown crystals. Dielectric measurements reveal that SR-method-grown DLM-doped ADP crystals have low dielectric loss. Crystalline perfection of the grown crystals is analyzed using HRXRD. Preliminary measurements indicate that the second harmonic generation efficiency of the doped crystals at a fundamental wavelength of 1064 nm is roughly 1.5 times greater than that of pure ADP. (C) 2009 Elsevier B.V. All rights reserved.