In this paper, the adsorption properties of wheat straw (WS) and corn straw (CS) for Cr(VI) and Cr(III) in solution were studied. The effects of adsorption time, pH of the solution, temperature, and initial concentration of metal ions on adsorption capacity were investigated. The adsorption mechanism was discussed. The results showed that the adsorption isotherms of WS and CS for Cr(VI) and Cr(III) satisfied the Langmuir equation. By fitting the Langmuir equation, the saturated adsorption capacity of WS for Cr(VI) and Cr(III) can reach 125.6 and 68.9 mg g −1 , and that of CS for Cr(VI) and Cr(III) can reach 87.4 and 62.3 mg g −1 , respectively. The adsorption kinetics conformed to the pseudo-second-order kinetic equation. The effect of temperature on the adsorption capacity was not significant. Physical diffusion and chemical adsorption coexist in the process of adsorption of metal ions by straws, and chemical adsorption is dominant, and the effect of physical diffusion on the chemical adsorption rate can be neglected. It can be seen from the experimental results that the treatment of chromium-containing wastewater by using cheap and easily available wheat straw and corn straw had a remarkable effect. The adsorbed straw could be completely desorbed and had excellent recyclability, indicating that the straws are ideal adsorbents.