A potentially useful semi-organic nonlinear optical single crystal of strontium bis (hydrogen l-malate) hexahydrate (SrLM) has been synthesized. Optically good quality bulk single crystal of SrLM was successfully grown by slow cooling technique and Sankaranarayanan—Ramasamy (SR) method. Transparent, colourless crystal of size 24mm×5mm×6mm with well defined morphology was grown by slow cooling method and 〈010〉-oriented unidirectional bulk single crystal of size 50mm length and 10mm diameter was grown by the SR method. The unit cell parameters and the morphology of SrLM single crystals were determined by single crystal XRD. The grown crystals were subjected to various characterization studies such as FTIR analysis, UV-visible spectrum, dielectric measurement, DTA, powder SHG test and microhardness studies.