Urea was grown from aqueous solutions with the organic additives by the slow evaporation method for obtaining an improved crystal size and enhanced nonlinear properties. The new material obtained was nonhygroscopic with remarkable morphological change compared to pure urea. The influence of the organic additives on the optical, structural, thermal and mechanical properties of urea were studied by UV in visible region, Fourier transform infra red spectroscopy, X-ray diffraction and microhardness studies by Vicker’s hardness test. The second order nonlinear optical property was examined by Kurtz powder technique and is measured using Nd:YAG laser at 1064 nm with a beam energy of 3.2 mJ/pulse. This material grown as a single crystal has a widespread application in the field of optoelectronics engineering and technology.