A cross-linked chitosan/(MnFe2O4) CCsMFO nanocomposite was prepared using co-precipitation methods and used as a nanomaterial to extract U(VI) and Th(IV) from an aqueous solution based on adsorption phenomena. The contact time of experiments shows a rapid extraction process within 30 min by the CCsMFO nanocomposite. The solution pH acts a critical role in determining qm value, where pH 3.0 was the best pH value to extract both ions. The pseudo-second-order equilibrium model illustrated the kinetics equilibrium modal extraction process. Adsorption isotherm of U(VI) at pH 3.0 by CCsMFO nanocomposite is an endothermic process. In contrast, the adsorption isotherm of Th(IV) at pH 3.0 by CCsMFO nanocomposite is an exothermic process. The reusability of CCsMFO nanocomposite was tested using basic eluents as suitable conditions for the chemical stability of CCsMFO nanocomposite; the reusability results show promising results for the removal of U(VI) adsorbed onto CCsMFO nanocomposite with 77.27%, after 12 h by Na2CO3 as eluent. At the same time, the reusability results show good reusability for removal of U(VI) adsorbed onto CCsMFO nanocomposite with 21.82%, after 8 h by EDTA as eluent.