Introduction of Hg2+ into an aqueous solution containing oligonucleotide-tethered gold nanoparticle probes and a linker oligonucleolide with a number of thymine-thymine (T-T) mismatches results in the formation of particle aggregates at room temperature with a concomitant colorimetric response. The high selectivity of this detection system is attributed to Hg2+-mediated formation of T-Hg2+-T base pairs as evidenced by an increase in a sharp melting temperature.