In this work, the mixture of methanol and zeolitic imidazolate framework (ZIF-8) was proposed for CO2 capture by adsorptive absorption at low temperatures. Methanol and ZIF-8 serve as absorption and adsorption functions, respectively. The solubility of CO2 in the different mixed absorbents (95 wt % methanol + 5 wt % ZIF-8, 90 wt % methanol + 10 wt % ZIF-8, and 85 wt % methanol + 15 wt % ZIF-8) at temperatures of (273.2, 258.2, and 243.2) K were measured using a low-temperature, high-pressure equilibrium cell. Moreover, a predictive thermodynamic model combining UNIFAC model and GCMC (grand canonical Monte Carlo) simulation together was used for predicting the CO2 solubility. The experimental and modeling results indicate that at low pressures the addition of ZIF-8 into methanol can increase the CO2 solubility; however, at high pressures the intensification of adding ZIF-8 on CO2 solubility is not so obvious. Additionally, the content of methanol in gas phase decreases significantly using the methanol and ZIF-8 mixture, which means that the volatile solvent loss at the top of separation column can be reduced by adsorptive absorption.