A fluorescent optical fiber sensor for the detection of mercury (Hg2+) ions in aqueous solutions is presented in this work. The sensor was based on a fluorophore-labeled thymine (T)-rich oligodeoxyribonucleotide (ON) sequence that was directly immobilized onto the tip of a tapered optical fiber. In the presence of mercury ions, the formation of T–Hg2+-T mismatches quenches the fluorescence emission by the labeled fluorophore, which enables the measurement of Hg2+ ions in aqueous solutions. Thus, in contrast to commonly designed sensors, neither a fluorescence quencher nor a complementary ON sequence is required. The sensor presented a response time of 24.8 seconds toward 5 × 10−12 M Hg2+. It also showed both good reversibility (higher than the 95.8%) and selectivity: the I0/I variation was 10 times higher for Hg2+ ions than for Mn2+ ions. Other contaminants examined (Co2+, Ag+, Cd2+, Ni2+, Ca2+, Pb2+, Mn2+, Zn2+, Fe3+, and Cu2+) presented an even lower interference. The limit of detection of the sensor was 4.73 × 10−13 M Hg2+ in buffer solution and 9.03 × 10−13 M Hg2+ in ultrapure water, and was also able to detect 5 × 10−12 M Hg2+ in tap water.