Trace detection of fluoride ion has gained increasing attention due to fluoride’s close association with biological and environmental processes. Herein, we construct a novel hybrid nanosystem consisting of carbon dots and curcumin for sensitive and selective sensing of F–. Carbon dots are synthesized by hydrothermal treatment of 2,3-diaminopyridine and selenourea in hydrochloric acid. This material is employed as the fluorescent indicator that exhibits intense blue and yellow emission with quantum yields of 12% and 33%, respectively. Curcumin, possessing an absorption peak at 532 nm, can significantly quench the yellow fluorescence of carbon dots through inner filter effect. Curcumin is also used to specifically recognize F–. When F– is added, the curcumin-F– complex generates, which leads to the hypochromatic shift of the absorption band from 532 to 430 nm. In such a case, the inner filter effect reduces, and yellow fluorescence of carbon dots recovers. Thus, a fluorescence turn-on sensor of F– is built based on the carbon dots/curcumin system. The limits of detection and quantitation are measured to be 0.39 and 1.30 μM, respectively. For real usage, the proposed method is applied to determinate F– in tap water and milk samples with relative standard deviations below 7.9%.