High fluoride concentration can cause many severe diseases and pose a certain threat to human health, to ensure the normal concentration in aqueous solution is within the specified threshold. Herein, a bimetallic Ce/Zr-MOFs with excellent adsorption performance was fabricated to eliminate the fluoride. The influences of reaction temperature, solution pH and co-existence ions on fluoride removal efficiency were examined. The outcomes showed that Ce/Zr-MOFs had a high adsorption performance. The adsorption kinetic and thermodynamic investigations indicate that the sorption procedure of fluoride ions conformed to the pseudo-second order model and the Langmuir model. The combination of XRD, XPS, and FTIR characterization reveals that the fluoride elimination mechanisms are electrostatic interactions and ion exchange.