The semi-organic nonlinear optical material of 5-(2-azaniumyl-2-carboxyethyl)-1H-imidazol-3-ium dimethanesulfonate has been grown as good quality single crystals through the Slow Evaporation Solution Growth technique (SEST). Single crystal XRD study of the titled compound was carried out to unfold the structural information. The study revealed that the grown crystal has a monoclinic structure under non-centrosymmetric space group. The Hirshfeld surface analysis and 2D fingerprint plots were employed to determine the intermolecular interaction in the crystal structure of the compound. Thermal properties of the compound were confirmed through TGA/DTA/DTG analysis and found that no significant weight loss of the compound appears up to 221 °C. In the DTA curve, the endothermic peak obtained at 182 °C, accounts for the decomposition of the compound. Whereas, the specific heat of the material was determined through DSC in which an exothermic peak is obtained at 181.86 °C. This peak represents the maximum specific heat of the material which comes out to be 16.845 J/g °C at 181.86 °C. The Heteronuclear chemical shift correlation (HETCOR) analysis based on 2D NMR spectroscopy was performed to determine the carbon-hydrogen bonding within the compound. UV-VIS- NIR spectroscopy was performed to find the energy band gap of the titled compound. The Stability of the material against highly intense laser was determined through the Laser damage threshold (LDT) value. The mechanical stability of the sample crystal was analysed through shock damage threshold (SDT) after the application of different shocks. With pre and post application of shocks, the Powder XRD of the sample was carried out. The SHG efficiency of the powdered sample was measured using Nd: YAG laser taking KDP as reference material.