The pure and semiorganic material of L-Histidine monohydrochloride dihydrate (LHMHC dihydrate) doped sodium acid phthalate (NaAP) single crystals were effectively grown from deionized water by slow evaporation solution technique. Single crystal X-ray diffraction is employed to know the precise information about the crystallographic structure and also the title materials are orthorhombic crystal system with space group B2ab. The interaction of various functional groups was recognized by FT-IR spectral study. The title materials are optically transparent and having a lower cut-off wavelength as 300 nm, thereby confirming the enhancement of nonlinear optical property and optical band gap of the pure and LHMHC dihydrate doped NaAP crystals have been determined as 3.5 eV and 4 eV by UV-Visible studies. The dielectric constant and dielectric loss of the pure and LHMHC dihydrate doped NaAP crystals decrease as the frequency of applied field increases at the end. The mechanical behaviors of the grown crystals were assessed by Vickers microhardness activities. The SHG efficiency of the grown crystals confirms NLO behavior of green colour emission to offer frequency doubling process for photoelectronic applications.