Dimethyl arsonic acid, the most common organic arsenic pollutant, is widely present in the environment and seriously threatens the safety of drinking water. Syntheses of magnetite, magnetic bentonite, and magnetic ferrihydrite via hydrothermal methods, and the magnetic composites were examined using XRD, BET, VSM, and SEM. SEM images revealed that many monodispersible pellets were attached to the surface of magnetic bentonite. The magnetic ferrihydrite contained abundant pores and had a rich pore structure, which expanded the specific surface area of the original magnetite. The specific surface areas of the magnetic bentonite and magnetic ferrihydrite were 65.17 and 220.30 m²·g⁻¹, respectively. The adsorption kinetics and adsorption isotherms of dimethyl arsonic acid on magnetic composites were studied. The adsorption of dimethyl arsonic acid on the magnetic composites conformed to the pseudo-second-order model and Freundlich isothermal adsorption model. By comparing the isotherms of the adsorption of dimethyl arsonic acid by the magnetic composites at pH values of 3, 7, and 11, respectively, it was found that the adsorption of dimethyl arsonic acid was the greatest at neutral pH of 7. The adsorption mechanism was analyzed via zeta potential determination, Fourier transform infrared spectroscopy (FT-IR), and X-ray photoelectron spectroscopy (XPS). The zeta potential results revealed that magnetic bentonite electrostatic activity occurred with dimethyl arsonic acid, and the magnetic ferrihydrite indicated a coordination complex with dimethyl arsonic acid. The XPS results revealed that the Fe–O bonds on the surfaces of the magnetic ferrihydrite had coordination complexation effects on the As-O of the dimethyl arsonic acid.