A multifunctional fluorescent and colorimetric receptor 1 ((E)-N′-((8-hydroxy-1,2,3,5,6,7-hexahydropyrido[3,2,1-ij]quinolin-9-yl)methylene)benzohydrazide) for the detection of both Al3+ and CN− in aqueous solution has been developed. Receptor 1 exhibited an excellent selective fluorescence response toward Al3+. The sensitivity of the fluorescent based assay (0.193 μM) for Al3+ is far below the limit in the World Health Organization (WHO) guidelines for drinking water (7.41 μM). In addition, receptor 1 showed an excellent detection ability in a wide pH range of 4–10 and also in living cells. Moreover, receptor 1 showed a highly selective colorimetric response to CN− by changing its color from colorless to yellow immediately without any interference from other anions.