In this study, polyacrylamide was coated onto Fe 3 O 4 to prepare novel polyacrylamide coated-Fe 3 O 4 magnetic composites (denoted as Fe 3 O 4 @PAM). The as-prepared composites were characterized by Fourier transferred infrared spectroscopy, X-ray diffraction, and thermo gravimetric analysis, and the results indicated that polyacrylamide was successfully coated on the surface of Fe 3 O 4 . And Fe 3 O 4 @PAM composites were applied as adsorbents to remove U(VI) from aqueous solutions and it could be separated by a simple magnetic separation method. The sorption isotherms were well fitted by the Langmuir sorption isotherms, and the maximum sorption capacity of Fe 3 O 4 @PAM for U(VI) at pH 5.0 was calculated to be 220.9mg/g. According to the XPS analysis of Fe 3 O 4 @PAM before and after U(VI) sorption, the nitrogen-containing functional groups on the surface of Fe 3 O 4 @PAM were responsible for U(VI) sorption. The U(VI) sorbed onto Fe 3 O 4 @PAM could be desorbed effectively in acid solutions, and the sorption capacity of regenerated sorbents could still maintain high level even after five cycles. The results showed that the Fe 3 O 4 @PAM composites were promising materials for the separation and enrichment of radionuclides from aqueous solution in environmental pollution cleanup.