Poly(n-vinyl-2-pyrrolidone)-stabilizedgold nanoparticles (PVP-Au-NPs) have been synthesized via a green-60 Co-Gamma radiolytic route and employed as a localized surface plasmon resonance (LSPR)-based optical sensor for estimation of trace quantities of Hg 2? ion in aqueous solutions. The in situ generated PVP-Au-NPs were characterized using UV-vis spectroscopy, transmission electron microscopy, and particle size analysis techniques. Reaction conditions were optimized to obtain uniformly dispersed PVP-Au-NPs with average particle size of 7.1 ± 1.6 nm (±s), which exhibited a narrow LSPR band at *527 nm. The decrease in LSPR band intensity of PVP-Au-NPs with increase in Hg 2? ion concentration was found to be linear in the Hg 2? ion concentration range of 0-100 nM. The LSPR-based PVP-Au-NPs optical sensor system was found to be selective for Hg 2? and independent of interference from other metal ions such as Ca 2?, Cu 2? , Cd 2? , and Fe 2? up to a concentration of 500 nM.