Potassium dihydrogen phosphate (KH2PO4; KDP) is a well known nonlinear optical (NLO) material for optoelectronic, laser technology and fiber optical communication device applications. In a view to yeild better device properties, l-Phenylalanine (l-Phe) aminoacid doped KDP (LKDP) crystals with different dopant concentrations (0.5 mol%, 1 mol% and 2 mol %) were grown by slow evaporation solution technique (SEST). The grown crystals were powdered of micron size crystallites and subjected to powder X-ray diffraction (PXRD). In PXRD spectra, a few peaks with increasing intensity were observed in LKDP crystals when compared to pure KDP, revealing the effect of incorporation of dopants in the crystalline matrix of KDP and the enhancement of growth rate along [100] direction. FT-IR spectrum confirms the incorparation of dopant in KDP crystalline matrix with the presence of different vibrational modes of assignments belongs to L-Phe. To study the crystalline perfection of pure and doped crystals, the high-resolution X-ray diffraction (HRXRD) was employed and the crystalline perfection was found to be reasonably good with relatively low values of FWHM. UV–Vis-NIR spectroscopy results show significant increase in optical transmission up to ~ 80% from ~ 60% (pure KDP) in the entire visible spectrum of l-Phe doped KDP at low doping concentration. However, it was decreased to ~ 70% when we increase the dopant concentration by 2 mol% and suggests that if we increase the dopant (l-Phe) concentration above an optimal value in KDP, the transmission decreases. The Photoluminescence (PL) spectrum reveals high crystalline perfection at low concentration of dopants as observed by the sharp peaks. The weak green emission peak for sample with higher dopant concentrations indicates the segregation of doped molecules at the structural grain boundaries as observed in the HRXRD studies. The mechanical strength of pure and doped KDP crystals with increasing dopant concentration has been studied and found that the hardness was increased slightly due to doping. The powdered sample of micron size particle made from as grown crystals were subjected to Kurtz powder technique to observe the relative second harmonic generation (SHG) efficiency in comparison with the pure KDP. These results reveal significant enhancement of SHG efficiency with increasing doping concentration up to 2 mol% in KDP crystals which is 1.31 times to that of pure KDP. © 2021, The Author(s), under exclusive licence to Springer Science+Business Media, LLC part of Springer Nature.