This research work reports the magnetic adsorption of fluoride from drinking water through silica-coated Fe3O4 nanoparticles. Chemical precipitation and wet impregnation methods were employed to synthesize the magnetic nanomaterials. Moreover, the synthesized nanomaterials were characterized for physicochemical properties through scanning electron microscopy, Fourier-transform infrared spectroscopy, and X-ray powder diffraction. Screening studies were conducted to select the best iron oxide loading (0.0–1.5 wt%) and calcination temperature (300–500 °C). The best selected nanomaterial (0.5Fe-Si-500) showed a homogenous FeO distribution with a 23.79 nm crystallite size. Moreover, the optimized reaction parameters were: 10 min of contact time, 0.03 g L−1 adsorbent dose, and 10 mg L−1 fluoride (F−) concentration. Adsorption data were fitted to the Langmuir and Freundlich isotherm models. The Qm and KF (the maximum adsorption capacities) values were 5.5991 mg g−1 and 1.869 L g−1 respectively. Furthermore, accelerated adsorption with shorter contact times and high adsorption capacity at working pH was among the outcomes of this research work.