The present study investigated fluoride removal by high-gradient superconducting magnetic separation (HGSMS) and paramagnetic adsorbents. FeAlOxHy adsorbents with different Fe/Al molar ratios were synthesized and characterized. The adsorption capacities of FeAlOxHy increased with increasing Al content. The FeAlOxHy were effectively separated in HGSMS, and approximately 87% of the fluoride was removed. Higher magnetic intensity, lower flow rate and finer steel wool are among the advantages of FeAlOxHy separated in HGSMS. The maximum desorption efficiency of fluoride adsorbed by FeAlOxHy was measured as 92.06%. A fluoride concentration time value of 40 was obtained using FeAlOxHy followed by the HGSMS process.