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We prepare oligothymonucleic acid (OTA) functionalized polyethylene (PE) film and evaluate its selective removal ability of mercury ions at ultra-low levels in aqueous solution. The selective binding of OTA with mercury ions is confirmed by fluorescence in situ hybridization (FISH). The quantitative results via cold-vapor atomic fluorescence spectrometry (CVAFS) indicate that OTA-functionalized PE film is able to remove mercury ions at the sub-ppb level selectively from aqueous solution, even with the coexistence of other metal ions at concentrations 250-fold or higher than that of mercury.