Against the backdrop of “carbon neutrality”, the green treatment of dye wastewater is particularly important. Currently, the adsorption method shows strong application prospects. Therefore, selecting efficient and recyclable adsorbents is of significant importance. TiO2 is an excellent adsorbent, but its difficult recovery often leads to secondary pollution. γ-Fe2O3-modified coal-series kaolin exhibits both excellent adsorption properties and rapid separation through magnetic separation technology. By utilizing the synergistic effects of both, TiO2/-γFe2O3 coal-series kaolin, magnetic adsorbent regeneration materials were prepared using coprecipitation method and characterized. The influencing factors of this functional material on the adsorption of Congo red dye and its regeneration performance are discussed. The experimental results indicated that the specific surface area, pore volume and Ms value of this functional material are 127.5 m2/g, 0.38 cm3/g, and 13.4 emu/g, respectively. It exhibits excellent adsorption characteristics towards Congo red, with an adsorption rate reaching 96.8% within 10 min, conforming to the pseudo-second-order kinetic model, and demonstrating Langmuir IV-type monolayer adsorption. After the adsorption of Congo red, magnetic separation shows superior efficiency. Furthermore, treatment of the adsorbed composite with EDTA allows for recycling, with adsorption rates still above 91% after three cycles, indicating an excellent regeneration capability.