We report here "aptatags," which consist of aptamer-modified silver nanoparticles (NPs) held together by an optical reporter. It is possible to use these materials to design a heterogeneous method for protein identification that takes advantage of the Raman signal enhancement by metallic nanostructures and the recognition capabilities of aptamers. Aptatags are formed by linking silver NPs with an organic dithiol molecule, followed by surface modification with thiolated single-stranded DNA (ssDNA) corresponding to the sequence of the aptamer probe. The sensing surface involves a silver layer containing the thiolated capturing aptamer and mercaptohexadecanoic acid to minimize nonspecific binding. The overall process provides excellent selectivity and sensitivity. Detailed characterization of the sensing surface by SERS maps and atomic force microscopy was carried out to understand how structural features lead to signal generation.