Single crystals of pure and amino acid (L-arginine) doped γ-glycine single crystals have been grown from aqueous solution by employing slow evaporation method. Morphological changes in different crystallographic planes were observed in the L-arginine doped γ-glycine crystals. Incorporation of L-arginine was confirmed qualitatively by FTIR spectroscopy. Powder X-ray diffraction was carried out to confirm γ-glycine and assess the single phase nature of the crystals. The lower cutoff wavelength was decreased by the influence of L-arginine in γ-glycine and this leads to an increase in the band gap. Nonlinear optical study revealed that L-arginine doping increases the SHG efficiency of the glycine crystal.