Elevated　fluoride　levels　in　drinking　water　pose　a　significant　challenge　to　human　health,　necessitating　affordable　and　effective　adsorbents　for　fluoride　removal.　This　study　presents　the　synthesis　of　a　Ce-Al　binary　metal　oxide　composite　adsorbent　supported　on　activated　carbon　(Ce-Al-O/AC)　for　the　defluoridation　of　drinking　water.　The　adsorbent,　employing　the　synergistic　bimetallic　effect,　demonstrates　robust　fluoride　removal　performance　across　a　wide　pH　range　of　4-10.　It　is　worth　highlighting　that　the　equilibrium　adsorption　capacity　reaches　17.97　mg　g−1　at　298　K　and　pH　6　within　2　h,　utilizing　an　adsorbent　dose　of　0.5　g　L−1　in　an　initial　10　mg　L−1　fluoride　solution.　The　phosphate　exerts　the　most　significant　influence　on　the　defluoridation　efficiency.　The　adsorption　kinetics　and　isotherms　align　with　the　pseudo-second-order　kinetics　model　and　Langmuir　isotherm　model,　respectively.　Moreover,　the　defluoridation　process　is　characterized　as　spontaneous　and　endothermic,　with　a　maximum　adsorption　capacity　of　31.65　mg　g−1　at　298　K.　Further　experimental　and　theoretical　evidences　reveal　that　fluoride　adsorption　is　primarily　driven　by　electrostatic　interactions　and　ion　exchange.　The　dynamic　adsorption　tests　coupled　with　economic　analyses　highlight　the　promise　of　Ce-Al-O/AC　as　a　cost-effective　and　efficient　adsorbent　for　practical　drinking　water　defluoridation.　©　2025　The　Royal　Society　of　Chemistry.