Eethylenediamine was grafted on metal-organic framework (MOF) material MIL-101(Cr) by solvothermal method, and the modified material used for adsorption of CO2 under atmospheric pressure. The effects of grafted amount of ethylenediamine and temperature on the structure morphology of the material and adsorption performance of CO2 were examined. The results showed that compared with unmodified MIL-101(Cr), the adsorption capacity of CO2 reached 2.43 mmol/g, gaining 14.6% increase after ethylenediamine modification at normal temperature and pressure. At the same time, the separation factor of CO2 with N2 by adsorption increased from 11 to 17, raising 55.6%. The modified material could be completely regenerated under the vacuum degree of 0.001 Pa at 80℃, indicating its good stability.