Maximum adsorption capacity of CNFs for U(VI) at pH 4.5 and 293 K was 52.63 mg/g. U(VI) sorption on CNFs at pH 4.0 was outer-sphere complexation by EXAFS analysis. Inner-sphere complexation/ co-precipitate dominated U(VI) adsorption at pH 7.0. U(VI) sorption can be satisfactorily fitted by surface complexation modeling.