In order to design better carbon capture materials, MIL-101 (Cr) was prepared using hydrothermal method, and then modified with different concentrations of choline chloride in a one-step method to enhance its CO2 adsorption capacity. The characterization and experimental results indicate that the modified ChCl-MIL-101(Cr) has significantly enhanced the adsorption capacity for CO2. Specifically, the 0.075-ChCl-MIL-101(Cr) has shown a 61.191% increase in adsorption capacity compared to the raw material. Moreover, the regenerated adsorption loss rate of the modified material is below 4%, which proves the permanence of the material synthesis.By simulating isotherms using Langmuir and Freundlich equations, the non-uniformity of surface bonding was obtained. Therefore, this study opens up a new avenue for designing choline chloride modified MOF based materials with advanced gas adsorption properties.