The　performance　of　a　Ce(III)-4,4′,4″-((1,3,5-triazine-2,4,6-triyl)　tris　(azanediyl))　tribenzoic　acid–organic　framework　(Ce-H3TATAB-MOFs)　for　capturing　excess　fluoride　in　aqueous　solutions　and　its　subsequent　defluoridation　was　investigated　in　depth.　The　optimal　sorption　capacity　was　obtained　with　a　metal/organic　ligand　molar　ratio　of　1:1.　The　morphological　characteristics,　crystalline　shape,　functional　groups,　and　pore　structure　of　the　material　were　analyzed　via　SEM,　XRD,　FTIR,　XPS,　and　N2　adsorption–desorption　experiments,　and　the　thermodynamics,　kinetics,　and　adsorption　mechanism　were　elucidated.　The　influence　of　pH　and　co-existing　ions　for　defluoridation　performance　were　also　sought.　The　results　show　that　Ce-H3TATAB-MOFs　is　a　mesoporous　material　with　good　crystallinity,　and　that　quasi-second　kinetic　and　Langmuir　models　can　describe　the　sorption　kinetics　and　thermodynamics　well,　demonstrating　that　the　entire　sorption　process　is　a　monolayer-governed　chemisorption.　The　Langmuir　maximum　sorption　capacity　was　129.7　mg　g−1　at　318　K　(pH　=　4).　The　adsorption　mechanism　involves　ligand　exchange,　electrostatic　interaction,　and　surface　complexation.　The　best　removal　effect　was　reached　at　pH　4,　and　a　removal　effectiveness　of　76.57%　was　obtained　under　strongly　alkaline　conditions　(pH　10),　indicating　that　the　adsorbent　has　a　wide　range　of　applications.　Ionic　interference　experiments　showed　that　the　presence　of　PO43−　and　H2PO4−　in　water　have　an　inhibitory　effect　on　defluoridation,　whereas　SO42−,　Cl−,　CO32−,　and　NO3−　are　conducive　to　the　adsorption　of　fluoride　due　to　the　ionic　effect.　©　2023　by　the　authors.