Single crystals of pure and crystal violet dye-doped L-Argininium bis dihydrogen phosphate were grown using slow evaporation technique. The crystalline nature and the structure parameters were confirmed by powder X-ray diffraction technique. Blue and red shifting hydrogen bonds were predicted by DFT on the basis of vibrational spectral (FT-IR & FT-Raman), AIM and NBO analyses. Bifurcated N[sbnd]H⋯O and O[sbnd]H⋯O intermolecular hydrogen bonds in LADP molecule were visualized by Hirshfeld surface. 13C and 1H NMR spectroscopy confirmed the structure of LADP. Doped LADP crystal shows enhancements in the wavelength and longer lifetimes as identified from photoluminescence spectra and decay analysis respectively. The high values of electron mobility and low value of λelectron reflect the applicability of LADP in OLED devices. Enhancement in nonlinear optical parameters in dye-doped LADP crystal was revealed from the Z-scan technique which shows its usefulness in the fabrication of NLO devices. © 2019 Elsevier B.V.