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Eutrophication caused by excessive discharging of phosphorus is a global water pollution problem. To further improve the phosphorus adsorption capacity of natural palygorskite and easy separation from liquid, magnetic thermal modified palygorskite nanocomposite (MTPG) was firstly fabricated and then characterized by XRD and SEM-EDS. The characterization results showed Fe₃O₄ in nano-diameters was prosperously immobilized on the surface of thermal modified palygorskite (TPG) calcinated at a temperature of 700 °C. Abundant nano-scale Fe₃O₄ loading almost doubled the specific surface area (SSA) of TPG. The adsorption of phosphate onto MTPG was highly pH-dependent and slightly influenced by ionic strength. According to the results from the Langmuir model, the maximum adsorptive quantity of 400.00 mg/g was counted at 298 K. The regeneration ratio was 80.98% after three regeneration cycles. The process of phosphate adsorption was confirmed to be an endothermic and spontaneous chemisorption. Thus, the cost-effective, excellent phosphate affinity, great magnetic recovery performance, and high adsorption capacity of MTPG had an enormous promising utilization on phosphate removal from aqueous solutions.