Single crystals of pure and Li + doped L-citrulline oxalate (LCO) crystals are grown successfully by slow evaporation technique. The effect of lithium doping on crystal properties has been studied. The samples are characterized by X-ray powder diffraction, TGA, FTIR, Raman and UV-Vis spectroscopic techniques. The presence of lithium in Li + doped LCO crystals is estimated using AES. The thermal stability and the optical transparency region are found to be enhanced for the doped samples. The second harmonic generation efficiency of the doped crystal has improved considerably compared to pure L-citrulline oxalate. Lithium doping can hence be considered as a simple and advantageous technique to improve the thermal, optical and non linear optical (NLO) properties of the LCO single crystals.