Excessive fluorine can cause a serious threat to human health. It is significant but challenging to develop a straightforward and rapid way to simultaneously detect and remove excess F − from water. Herein, we presented a three-dimensional (3D) hierarchical UiO-66-NH 2 nanoparticle/γ-AlO(OH) nanowire hybrid synthesized by a facile biotemplate route for simultaneous detection and removal of F − from water. We elaborately assembled two kinds of materials in a bioinspired 3D hierarchical structure as a functional unit to achieve detection and removal of dual functions. The outer UiO-66-NH 2 nanoparticles served as a fluorescent sensor to detect and capture F − via a strong fluorescence enhancement effect caused by the electron transfer from F − and γ-AlO(OH) and acted as the capture unit of F − . The inner γ-AlO(OH) nanowire layer served as a F − absorbent through ion exchange between F − and γ-AlO(OH). The resulting UiO-66-NH 2 nanoparticle/γ-AlO(OH) nanowire hybrid displayed excellent selectivity and sensitivity for F − detection (the detection range was 0−5 mM and the limit of detection was as low as 0.77 μM) and high capacity for F − removal (the maximum equilibrium adsorption capacity q max was as high as 87.0 mg g −1 ). This dualfunction material provided a strategy for simultaneously selective sensing and efficient removal of anionic pollutants from water.