NLO active 2-Amino-5-methylpyridinium-2-hydroxy-5-chlorobenzoate single crystals have been successfully grown by standard slow evaporation technique. The solubility and metastable zone width for crystal have been studied. The compound crystallizes in a noncentro symmetric space group which is prerequisite for SHG generation. The UV-visible absorption and transmittance spectra have been recorded for the grown crystal and optical band gap is also calculated. Fourier transform infrared (FT-IR) and Raman spectroscopic studies also have been performed for the identification of different modes present in the compound. The 1H and 13C NMR spectra of as grown AMPHCB crystal have been recorded to identify the existence of particular nuclei in a complex. The relative SHG efficiency of the material is investigated. The phase matching property of the crystal is studied through the SHG dependence of average particle sizes. The dielectric study shows that the dielectric constant decreases with increase in frequency. Hardness study revealed the soft nature of the crystal. Besides, the crystal has been subjected to TG, DTA and DSC analysis. Quantum chemical calculations for the title compound were performed.