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A three-dimensional hierarchically structured flowerlike zeolite was synthesized using naturally occurring nanohalloysite (HNT) by hydrothermal methods. Halloysite a hydrated aluminum silicate with nanohollow morphology, microporosity, and environmentally friendly properties was chosen to be the sole precursor. The morphology and structure of the composite that was prepared was characterized using XRD, FT-IR, BET, TG, SEM, HRTEM, and NMR. SEM and HRTEM images indicated that the synthesized zeolite has a flowerlike hierarchical structure, with well-defined edges and uniform pore channels. FT-IR and NMR spectra indicated that different species of silicon and aluminum were present in the synthesized zeolite. The zeolite was applied in fluoride (F-) removal from aqueous solutions. Single-factor studies, including the initial concentration of F-, initial adsorbent concentration, and the effect of pH value on the adsorption properties, were investigated to evaluate the removal behavior of F- by the zeolite. The zeolite exhibited strong adsorption properties for fluoride ions (F-), with an adsorption capacity up to 161 mg g-1. The pseudo-second-order kinetics and Freundlich models were the best fit to the kinetics and isotherm experimental data, respectively.