In this work, illite was used to support zerovalent iron nanoparticles to remove 238 U in aqueous solutions. Compared to nZVI, I-nZVI shows high stability and removal efficiency. Removal process of U on I-nZVI can be concluded into four stages in illite dominated zone, Fe 0 released zone, ferrous dominated zone and reaction equilibrium zone. The study shows that illite is a good dispersant and stabilizer which decreases the aggregation of nZVI and improves the activity of Fe 0 . Removal capacity of U on I-nZVI achieves 1.79 lg/mg. I-nZVI is an efficient and promising remediation material for waste-soluble uranium compounds.