A nano-scale magnesium oxide (NS-MgO)-based adsorbent was developed for the remediation of fluoride-contaminated groundwater. Magnesium nitrate was used as the precursor, and the NS-MgO was synthesized via a solvothermal method. The resulting material exhibited spherical and crystalline structures, with a specific surface area of 4.2 m2/g and an average particle diameter of 20.4 nm. Adsorption studies revealed that the material followed the Freundlich isotherm and pseudo-second-order kinetic model, indicating that chemisorption was the dominant mechanism. The rate constant was determined to be 1.36 × 10−3 1/min, and the adsorption capacity was 227.3 mg/g·min at an initial fluoride concentration of 100 mg/L. Initially, monolayer adsorption was dominant; however, as the process progressed, multilayer adsorption became prevalent, thereby increasing the overall adsorption capacity. Higher concentrations of hydroxide, phosphate, and carbonate were observed to decrease the fluoride removal efficiency because of sorption sites competition with anions possessing similar electronic characteristics. The fluoride removal mechanism primarily involved two chemical pathways: (1) the formation of magnesium hydroxide through the reaction of MgO with water, and (2) the substitution of hydroxide ions by fluoride ions, resulting in the formation of magnesium fluoride precipitates [Mg(OH)