Single crystals of pure and L-threonine added tartaric acid (LT/TA), organic nonlinear optical (NLO) materials were grown from their respective aqueous solution by slow evaporation method. The crystalline nature of the grown crystals was confirmed by powder X-ray diffraction analysis (XRD). UV-Vis-NIR absorption and transmission spectra revealed that the lower cut-off wavelength was around 281 nm and the crystals exhibited high transmission over visible and near IR region. The presence of the functional groups such as O–H, C–H, C–O, C=O in the grown crystals was confirmed by FT-IR analysis. CHN analysis was carried out to confirm the presence of L-threonine in the grown crystals. Microhardness study on the crystals revealed that the hardness number Hv increased with the applied load. The growth pattern of the crystals were analyzed through etching analysis from which the etch patterns in the shape of ‘step-triangle’ were observed. The second harmonic generation (SHG) properties of pure and L-threonine doped tartaric acid crystals were confirmed by Kurtz-Perry powder technique.