Phosphorus　removal　is　essential　to　avoid　eutrophication　in　water　bodies.　Layered　double　hydroxides　(LDHs)　are　widely　used　to　scavenge　phosphate　through　intercalated　ion　exchange　or　surface　complexation.　Moreover,　LDHs　have　attracted　increasing　attention　as　electrode　modifiers　for　supercapacitors.　Researchers　have　begun　to　re-delve　the　electrosorption　technology　according　to　the　fundamental　principle　of　electrical　double　layers.　Herein,　we　propose　a　new　phosphate　removal　method　inspired　by　the　adsorption　characteristic　and　electrical　double-layer　capacitive　properties　of　LDHs　through　electrosorption　via　capacitive　deionization.　We　present　a　series　of　experiments　to　study　the　enhanced　phosphate　removal　under　an　electric　field　via　multiple　mechanisms　on　the　MgAl-LDHs/AC　electrode.　The　uptake　of　phosphate　by　MgAl-LDHs/AC　was　investigated　as　a　function　of　phosphate　concentration,　applied　voltage,　electrode　materials,　and　temperature.　The　MgAl-LDHs/AC　electrode　possessed　a　salt　removal　capacity　of　67.92　mg　PO43−·g−1　(1.2　V,　250　mg·L−1　KH2PO4,　30　°C).　The　electrosorption　kinetics　of　phosphate　ions　onto　the　capacitive　deionization　electrode　followed　the　pseudo-second-order　kinetics　model　rather　than　the　pseudo-first-order　kinetics　model.　Furthermore,　the　adsorption　isotherms　of　phosphate　on　the　MgAl-LDHs/AC　electrode　fitted　the　Freundlich　model　better　than　the　Langmuir　model.　The　proposed　method　could　be　used　for　phosphate　removal.　©　2019　Elsevier　B.V.