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[Display omitted] Bimetal oxide is a popular defluorinating material. Hexadecyl trimethyl ammonium bromide (CTAB) as a surfactant successfully synthesizes a novel lanthanum-zirconium phosphate to remove fluorine from groundwater. Lanthanum-zirconium phosphate at a Zr/La molar ratio of 2 exhibited a specific surface area of 455.14 m2/g with a wide pore size, which was achieved by incorporating lanthanum into materials and removing CTAB through calcination. The maximum fluoride adsorption capacity is 109.17 mg/g, which is tenfold that of mesostructured zirconium phosphate. Specifically, analysis revealed that mZrP and LamZrP2-1 were amorphous, which is consistent with HAADF-STEM. The fluoride adsorption fitted well with the pseudo-second-order equation model and Langmuir isotherm mode. LamZrP2-1 had potent anti-interference ability without PO43-. Moreover, LamZrP2-1 was reusable for at least six cycles of adsorption–desorption with little influence. The adsorption mechanism of fluoride was discussed by X-ray photoelectron spectroscopy (XPS), nuclear magnetic resonance spectroscopy (NMR) analysis, and Fourier transform infrared (FTIR) spectroscopy. Fluoride was captured by LamZrP2-1 via charge attraction, ligand exchange of different bond strengths, and ion exchange. Lanthanum-zirconium phosphate is important not only in the research and development of bimetal oxides but also in the treatment of groundwater for fluoride removal. [ABSTRACT FROM AUTHOR]