Developing green and functional adsorbents for the removal of inorganic pollutants from industrial wastewater is still a great challenge. Activated carbons (ACs) are promising eco-friendly materials for adsorption applications. This study reports on the preparation and functionalization of AC and its application for fluoride removal from water. Activated carbon was prepared from date stems, and the material was employed as a support for different modifications such as incorporation of Al(OH)3, in situ dispersion of aluminum particles (Al0) and grafting of 3-(aminopropyl)triethoxysilane (APTES). The resulting functional adsorbents were fully characterized by Fourier transform infrared spectroscopy, scanning electronic microscopy, energy dispersive X-ray fluorescence, X-ray diffraction, differential scanning calorimetry and zeta potential analysis. The results evidenced successful surface modifications. All adsorbents had affinity for the removal of fluoride ions (F−). The highest F− removal rate was up to 20 mg g−1 for AC-Al(OH)3. Removal of fluoride ions obeyed Langmuir isotherms and a second-order kinetic model, and reached 99% uptake. The AC-Al(OH)3 adsorbent was successfully used to treat a groundwater solution contaminated by fluoride ions. These results open an interesting avenue for developing eco-friendly functionalized AC for adsorption applications.