Adsorption of U(VI) from aqueous solution by cross-linked rice straw(CRS) was studied with batch experiments. The adsorbent was characterized by Fourier transform infrared spectroscopy (FT-IR). The effect of contact time, initial pH, temperature, adsorbent amount and initial U(VI) concentration was investigated. Langmuir, Freundlich and Dubinin–Radushkevich (D–R) adsorption isotherms and two kinetic models of pseudo-first-order and pseudo-second-order were used to describe the adsorption process. The result showed that the adsorption process was highly pH dependent and the favorable initial pH was 5.0. The adsorption process was rapid within first 60 min and equilibrium reached at 100 min. The adsorption process could be well defined by the Langmuir isotherm and pseudo-second-order equation, which indicated that the chemical adsorption was the rate-limiting step. The thermodynamic parameters (∆H°, ∆S°, ∆G°) of the adsorption system were also calculated. The negative value of ∆H° and ∆G° indicated that the reaction was endothermic and spontaneous in nature. All the above suggested that CRS has considerable potential for the removal of U(VI) from aqueous solution.