A new phosphorescent iridium(III) complex, bis[2',6'-difluoropheny1-4-formylpyridinato-N,C4']iridium(III) (picolinate) (IrC), was synthesized, fully characterized by various spectroscopic techniques, and utilized for the detection of CN- on the basis of the widely known hypothesis of the formation of cyanohydrins. The solid-state structure of the developed IrC was authenticated by single-crystal X-ray diffraction. Notably, the iridium(III) complex exhibits intense red phosphorescence in the solid state at 298 K (Phi(PL) = 0.16) and faint emission in acetonitrile solution (Phi(PL) = 0.02). The cyanide anion binding properties with IrC in pure and aqueous acetonitrile solutions were systematically investigated using two different channels: i.e., by means of UV-vis absorption and photoluminescence. The addition of 2.0 equiv of cyanide to a solution of the iridium(III) complex in acetonitrile (c = 20 mu M) visibly changes the color from orange to yellow. On the other hand, the PL intensity of IrC at 480 nm was dramatically enhanced similar to 5.36 x 10(2)-fold within 100 s along with a strong signature of a blue shift of the emission by similar to 155 nm with a detection limit of 2.16 X 10(-8) M. The cyanohydrin formation mechanism is further supported by results of a H-1 NMR titration of IrC with CN-. As an integral part of this work, phosphorescent test strips have been constructed by impregnating Whatman filter paper with IrC for the trace detection of CN- in the contact mode, exhibiting a detection limit at the nanogram level (similar to 265 ng/mL). Finally, density functional theory (DFT) and time-dependent density functional theory (TD-DFT) calculations were performed to understand the electronic structure and the corresponding transitions involved in the designed phosphorescent iridium(III) complex probe and its cyanide adduct.