A novel electrospun Fe3O4@SiO2@APTES/PVA nanofiber adsorbent for U(VI) sorption was synthesized and characterized by FTIR, SEM, BET and TG analyses. The effects of pH, nanoparticles content, adsorbent dose, contact time, initial U(VI) concentration, temperature and co-existing ions were studied in batch experiments. The sorption affinity of metal ions onto adsorbent was U(VI) > Cu(II) > Cd(II) > Pb(II) > Ni(II) > Th(IV). The kinetic and isotherm data were accurately described by the double-exponential and Langmuir model, with a maximum sorption capacity of 68.96 mg/g with a pH of 5. Thermodynamic parameters were evaluated to understand the nature of sorption process. The reusability of adsorbent was determined after five sorption-desorption cycles.