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In recent years there has been excessive progress in the 'green' chemistry approach for the synthesis of gold and silver nanoparticles. Bimetallic nanoparticles have gained special significance due to their unique tunable optical properties. Herein we report a facile one-pot, ecofriendly synthesis of Au-Ag bimetallic core-shell nanoparticles using gripe water as reducing as well as stabilizing agent. The as-synthesized Au-Ag nanoparticles are characterized using UV-Vis spectroscopy to determine the surface plasmon resonance, and using transmission electron microscopy to study the morphology and the particle size. The optical nonlinearity of the bimetallic nanoparticles investigated by z-scan technique using femtosecond Ti:sapphire is in the order of 10 9 . The nonlinear optical parameters such as the nonlinear refractive index n 2 , nonlinear absorption coefficient β and the third order nonlinear susceptibility χ 3 are measured for various wavelengths from 700 nm to 950 nm. The Au-Ag nanoparticles are also used in surface enhanced Raman spectroscopic studies to enhance the Raman signals of rhodamine 6G.