A simple method was used to synthesize magnetic xanthate-modified chitosan/polyacrylic acid hydrogels that were used to remove heavy metal ions from an aqueous solution. Xanthate modification of chitosan significantly improved adsorption performance: individual adsorption capacities of the hydrogel for Cu(II), Cd(II), Pb(II), and Co(II) ions were 206, 178, 168, and 140 mg g−1, respectively. The magnetic hydrogels had good regeneration ability and were effectively separated from the solution by use of a magnet. Adsorption kinetic data showed that the removal mechanism of heavy metal ions from the solution by magnetic hydrogels occurs mainly by chemical adsorption. The equilibrium adsorption isotherms were well-described by the Freundlich and Langmuir equations. Positive values were found for the Gibbs standard free energy and enthalpy, indicating an increase in the disorder at the solid–liquid interface during adsorption. Magnetic xanthate-modified chitosan-based hydrogels that exhibit high adsorption efficiency, regeneration, and easy separation from a solution have broad development prospects in various industrial sewage and wastewater treatment fields.