Capacitive　deionization　(CDI)　is　a　promising　technology　for　removing　phosphate　from　wastewater.　Its　practical　implementation　is　however　hindered　by　the　constraints　on　the　electrode　materials.　To　boost　the　adsorption　capacity,　phosphate　selectivity,　and　cost-effectiveness　of　the　electrode,　this　study　proposed　a　composite　electrode　blending　Lanthanum-based　layered　double　hydroxide　(Ca-La　LDH)　and　activated　carbon　(AC).　It　capitalizes　on　the　synergistic　effects　of　electric　double　layer　capacitance　(EDLC)　of　AC　and　the　diffusion-controlled　charge　storage　(pseudocapacitive　behavior)　of　Ca-La　LDH.　By　optimizing　the　mass　ratios　of　the　constituents　and　the　electrode　material　loading　capacities,　the　composite　electrode　AC/Ca-La　LDH-5020　was　developed,　which　contains　20　mg　of　50　wt%　Ca-La　LDH.　This　composition　achieved　a　remarkable　phosphate　adsorption　capacity　of　34.8　mg　P　/g　and　a　low　energy　consumption　of　0.0051　kWh/g　P　in　constant　voltage　(CV)　mode.　It　represented　a　241　%　increase　in　adsorption　capacity　(mg　P/g)　and　71　%　decrease　in　specific　energy　consumption　(kWh/g　P)　compared　to　the　electrode　made　solely　of　AC.　Particularly　the　moderate　inclusion　of　Lanthanum　contributes　to　its　cost-effectiveness.　Moreover,　further　studies　extensively　examined　the　impacts　of　electrical　driving　force,　including　applied　voltage　in　constant　voltage　(CV)　mode　and　applied　current　in　constant　current　(CC)　mode,　on　the　phosphate　removal　efficiency.　The　composite　electrode　remained　stable　performance　with　the　presence　of　the　high　content　of　coexisting　anions　(e.g.，Cl−，SO42−,　HCO3−,　NO3−),　obtaining　high　selectivity　coefficient　of　phosphate　over　other　anions.　This　study　highlighted　the　practical　potential　of　AC/Ca-La　LDH　composite　electrode　for　advancing　CDI　technology　for　phosphate　removal　in　an　efficient,　energy-saving　and　cost-effective　manner.　©　2024　Elsevier　B.V.