Because of the extreme toxicity of cyanide anions, a great deal of effort has been invested in developing probes that use colorimetric and fluorometric methods to detect them. To date, most of the current optical probes require the use of organic solvents or a mixture of organic solvents and water. Upconversion nanophosphors (UCNPs) can serve as excellent emitters as a result of their sharp emission peaks and simple control of the emission wavelength. Here, the fabrication of hybrid material composed of iridium complex and UCNPs to detect cyanide anions selectively in pure water is described. In addition to the colorimetric detection, the upconversion luminescence emission can serve as a detection signal based on an effective luminescent resonance energy transfer (LRET) process within the hybrid nanoparticles.