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Here, we report a highly sensitive and reliable surface enhanced Raman scattering (SERS)-based immunoassay using bimetallic alloy Ag@Au hollow dual-rim nanorings (DRNs) where two hollow nanorings with different diameters are concentrically overlapped and connected by thin metal ligaments, forming circular hot-zones in the intra-nanogaps between the inner and outer rims. Pt DRNs were first prepared, and then Ag was deposited on the surface of the Pt skeleton, followed by Au coating, resulting in alloy Ag@Au hollow DRNs. The chemical stability of Au and the high optical properties of Ag are incorporated into a single entity, Ag@Au hollow DRNs, enabling strong single-particle SERS activity and biocompatibility through surface modification with thiol-containing functionalities. When Ag@Au hollow DRNs were utilized as nanoprobes for detecting human chorionic gonadotropin (HCG) hormone through a SERS-based immunoassay, a very low limit of detection of 10 pM with high reliability was achieved, strongly indicating their advantage as ultrasensitive SERS nanoprobes.