Herein,　we　used　a　one-pot　method　to　fabricate　a　novel　MOF-on-MOF　adsorbent,　namely　MOF(Zr)-on-MOF(Ce).　The　adsorbent　demonstrated　a　high　maximum　fluoride-ions　capture　capacity　of　164.47　mg　g-1.　The　morphology,　elemental　distribution,　pore　size　distribution,　and　thermal　stability　were　studied　using　SEM-EDS,　XRD,　BET,　and　TGA.　The　influence　of　the　temperature,　solution　pH,　fluoride　concentration,　and　coexisting　ions　was　explored　using　intermittent　experiments.　The　results　suggested　that　MOF(Zr)-on-MOF(Ce)　had　a　fast　capture　rate　for　fluoride.　MOF(Zr)-on-MOF(Ce)　maintained　an　excellent　fluoride　removal　performance　over　a　wide　pH　range　with　an　initial　fluoride　concentration　of　20　mg　L-1.　The　optimal　effect　was　obtained　at　a　pH　of　4,　but　a　high　removal　efficiency　of　94%　was　maintained　even　at　a　pH　of　9.　Interference　experiments　showed　that　only　the　PO43-　had　an　adverse　inhibition　influence.　The　field　experiments　demonstrated　that　MOF(Zr)-on-MOF(Ce)　can　keep　the　safety　threshold　levels　of　fluoride　in　drinking　water.　The　Langmuir　and　pseudo-second　order　kinetic　models　were　well　fitted　for　the　defluoridation　process,　demonstrating　that　the　adsorption　of　fluoride　ions　on　MOF(Zr)-on-MOF(Ce)　was　dominated　by　monolayer　chemisorption.　With　the　further　characterization　and　kinetic　thermodynamic　studies　indicates　that　the　removal　mechanism　involves　ion　exchange,　electrostatic　interactions　and　complexation　effect.