Fluoride and cyanide contamination in drinking water imposes detrimental impacts on human health above their permissible limits. Hence, the quantitative detection of these colourless water-soluble toxins has attracted attention. Even though a plethora of chemosensors have been reported so far for the detection of fluoride and cyanide from various matrices, still their applicability is limited to a few examples. Nevertheless, recent advances in the syntheses of coumarin derivatives have shown significant impact on fluoride and cyanide detection. Therefore, this present review provides a brief overview of the application of coumarin-coupled molecular scaffolds towards the detection of perilous fluoride and cyanide along with their sensing mechanisms in order to develop more innovative, simple, sensitive, real-time responsive and cost-effective coumarin-based supramolecular chemosensors to promote next generation approaches towards the ultra-trace quantitative detection of these toxic anions.