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Introduction of Hg²⁺ into an aqueous solution containing oligonucleotide-tethered gold nanoparticle probes and a linker oligonucleotide 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.