The optical and colorimetric properties of a new chemosensor 4-((2,4-dichlorophenyl) diazenyl)-2-(3-hydroxypropylimino)methyl)phenol (L) for cyanide ions were investigated by the naked-eye detection and UVevis spectroscopy. This receptor reveals visual changes toward CN À anions in aqueous media. No significant color changes were observed upon the addition of any other anions. The cyanide recognition properties of the receptor through proton-transfer were monitored by UVevis titration and 1 H NMR spectroscopy. The binding constant (K a ) and stoichiometry of the formed hosteguest complex were calculated by the BenesieHildebrand (BeH) plot and Job's plot method, respectively. The detection limit of the probe towards CN À was 1.03 Â 10 À6 mol L À1 , which is lower than the maximum value of cyanide (1.9 Â 10 À6 mol L À1 ) permitted by the World Health Organization in drinking water. Thus, this chemosensor was sensitive enough to detect cyanide in aqueous solutions. 1 H NMR experiments were conducted to investigate the nature of interaction between the receptor and CN À anions. Notably, the designed sensor can be applied for the rapid detection of cyanide anions in the basic pH range and also under physiological conditions, for practical purposes for a long duration. The sensing behavior of the receptor was further emphasized by computational studies. Quantum-chemical calculations and molecular studies via Density Functional Theory (DFT) were carried out to supplement the experimental results.