Ammonium dihydrogen phosphate (ADP) single crystals along with the incorporated 0.5 and 1% L-lysine, an organic molecule which possesses a good nonlinear response, were grown with the vision to meet the requirements of the optoelectronic industry. The inclusion of the L-lysine molecule in the crystal was confirmed by the XRD and EDX. The experiment not only confirms the inclusion level of the impurity but also the capability of the amino acid molecule to bond hydrogen within the crystal facet. A minor decrease in lattice parameters was reported for all ADP: L-lysine crystals compared with pure ADP. The structures of the grown crystals were identified as tetragonal with the space group I42d by the single-crystal XRD analysis. Vibrational signatures and functional groups were confirmed using FTIR spectroscopy. The thermal stability and decomposition temperatures of 0.5 and 1% L-lysine-added crystals were measured by TG/DTA and found to be 203 °C and 207 °C, respectively. The UV–visible transmission spectra prove a higher transparency for doped crystals as compared to pure crystals; therefore, these doped crystals can be considered the best option for the frequency doubling process in a broad range of visible and near-IR spectra. The improved hardness of the doped crystals was confirmed by the Vickers hardness data. The nonlinear optical (NLO) behaviour investigated using a second-harmonic generation (SHG) technique, indicating an efficient quadratic nonlinear coefficient of ADP: Lysine crystals at a 1064 nm initial wavelength, shows about 1.5-fold higher efficiency compared with undoped ADP.