Gold-silver core-shell nanoparticles (Au@Ag NPs) were prepared by two successive reductions in a seed-growth method. The Au@Ag NPs are used as both a colorimetric and Raman spectroscopic probe for ultrasensitive determination of H2O2 and glucose. It is found that H2O2 (as produced from glucose by the action of glucose oxidase) can directly oxidize and gradually corrode the silver shell of the Au@Ag NPs. This results in a drop in the surface plasmon resonance absorbance at 400 nm, and the color of the solution changes from brownish yellow to purple. Without adding any additional chromogenic agents, the color change can be visually observed and detected photometrically. Silver NPs also are an excellent surface-enhanced Raman scattering (SERS) substrate. Due to corrosion of the silver shell, the SERS intensity (measured at 1083 cm−1) gradually decreases with increasing glucose concentration. The detection limits are 300 nM of glucose for the colorimetric assays, and 20 nM for the SERS assay.