The high concentration of fluoride ions in industrial wastewater poses a threat to both human safety and the ecological environment. In this paper, three types of magnetic NiO nanomaterial (MNN) with nickel–iron ratios of 3:1, 2:1, and 1:2 were successfully prepared using the electrodeposition technique to eliminate fluoride ions (F−) from industrial wastewater. The surface morphology, phase composition, and chemical structure of the nanomaterials were analyzed using scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray diffraction (XRD). The results demonstrate the MNN material’s exceptional adsorption capabilities for fluoride ions (F−) at a nickel–iron ratio of 3:1, with a maximum adsorption capacity of up to 58.3 mg/g. The adsorption process of fluoride on the MNN material was further examined using Langmuir and pseudo-second-order kinetic models, revealing predominantly monolayer adsorption and chemisorption characteristics. When the amount of FeSO4•9H2O added is minimal, only the distinctive peaks of NiO are visible in the product’s spectrum. However, as the Ni/Fe ratio decreases, characteristic peaks of Fe3O4 crystals begin to appear and gradually intensify, indicating an increase in Fe3O4 content within the MNN material. Additionally, the pH level significantly affects the adsorption of fluoride ions (F−) onto the MNN material, with the highest adsorption capacity observed at pH 7.