Single crystal of guanidinium l-monohydrogen tartrate (GuHT) was grown by slow evaporation technique and was characterized by single crystal X-ray diffraction to confirm its crystal structure. UV–vis spectral study reveal that the GuHT crystal is optically transparent and its band gap was estimated from the transmittance data. The laser induced surface damage threshold study was carried out for the grown crystal using Nd:YAG laser. The second harmonic generation (SHG) nonlinearity of the grown crystalline sample was measured by Kurtz and Perry powder technique. The optimized molecular geometry, first order hyperpolarizability, dipole moment and polarizability of GuHT were obtained by density functional theory (DFT) using B3LYP/6-31G (d,p) level of basis set. The thermodynamic functions of the title compound was computed. The HOMO–LUMO energy gap explains the charge transfer interactions that take place within the molecule.