Long-term consumption of drinking water that contains excessive amounts of fluoride can endanger human health; therefore, the preparation and application of a high-efficiency defluorination adsorbent for advanced purification of drinking water are of significant interest. This study presents a metal-organic framework adsorbent (MIL-96(Al)) with the granular structure of rice, which was generated by hydrothermal reaction. The specific surface area of MIL-96(Al) was ~220 m2 g-1, and it showed a good thermal stability. Several experiments were conducted wherein conditions, including adsorbent dosage, initial concentration, pH, and coexisting anions, were varied to understand the defluorination performance of the material. Results showed that pH (6–9) and coexisting anions had little effect on the removal efficiency of fluoride. The adsorption isotherm can be described by the Langmuir model, and the theoretical fluoride adsorption capacity of MIL-96(Al) was up to 42.19 mg Fg-1 at 298 K, which is much higher than that of the commonly used activated alumina. The adsorption process of fluoride is endothermic and follows pseudo second-order kinetics. In addition, MIL-96(Al) was shown to still achieve ~61.8% of the adsorption capacity after seven regenerations. This study shows that MIL-96(Al) is a good application prospect and could be widely used to remove fluoride from water.