A mesoporous UiO-66-NH2aerogel is prepared via a straightforward sol-gel method without using any binders or mechanical pressures, in which the amine groups are directly introduced into the matrix by using 2-aminoterephthalic acid. The novel UiO-66-NH2aerogel also exhibits high specific surface area and mesopore-dominated structure, implying its highly potential use in CO2adsorption. For ulteriorly investigating the effect of amine loading on the CO2adsorption ability, a series of UiO-66-NH2aerogel with different amino content is fabricated by changing the ligand/metal molar ratio. When the molar ratio is 1.45, the CO2adsorption capacity reaches the optimum value of 2.13 mmol·g–1at 25 °C and 0.1 MPa, which is 12.2% higher than that of pure UiO-66 aerogel. Additionally, UiO-66-NH2-1.45 aerogel also has noticeable CO2selectivity against N2and CH4as well as good regeneration stability. Such results imply that it has good application prospect in the field of CO2adsorption, and also contains the potential to be applied in catalysis, separation and other fields.