A water-soluble fluorescent probe (C-GGH) was used for the highly sensitive and selective detection of cyanide (CN−) in aqueous media based on the displacement strategy. Due to the presence of the recognition unit GGH (Gly-Gly-His), the probeC-GGH can coordinate with Cu2+and consequently display ON-OFF type fluorescence response. Furthermore, thein situformed nonfluorescentC-GGH-Cu2+complex can act as an effective OFF-ON type fluorescent probe for sensing CN−anion. Due to the strong binding affinity of CN−to Cu2+, CN−can extract Cu2+fromC-GGH-Cu2+complex, leading to the release ofC-GGH and the recovery of fluorescent emission of the system. The probeC-GGH-Cu2+allowed detection of CN−in aqueous solution with a LOD (limit of detection) of 0.017 μmol/L which is much lower than the maximum contaminant level (1.9 μmol/L) for CN−in drinking water set by the WHO (World Health Organization). The probe also displayed excellent specificity for CN−towards other anions, including F−, Cl−, Br−, I−, SCN−,PO43-,N3-,NO3-, AcO−,SO42-, andCO32-.