Proper amount of fluorion is very important to human health, but excessive fluorion is harmful. Therefore, the content of fluorion in tap water is strictly required to be controlled within a certain range. Here, we propose the first colorimetric and fluorescence enhanced sensor to detect fluorion with high selectivity. The classic MOF material UiO-66 is combined with fluorescent dye FITC to form a nano-system. When there is fluorion, which will be combined with UiO-66 and FITC, respectively, to achieve colorimetric and fluorescence enhancement. It has a good linear relationship in the range of 2–150 μM (0.038–2.85 ppm), and has been applied to the detection of actual water samples. The field visual detection of fluoride ion is realized, and the application of MOF in the field of fluorescence sensing is broadened.