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In the cement industry, utilization of a sustainable binder that has a lower energy consumption and carbon dioxide (CO2) emission than Portland cement is becoming increasingly important. Air lime is a binder that hardens by absorbing CO2 from the atmosphere, and its raw material, hydrated lime, is manufactured at a lower temperature (around 900 degrees C) than cement (around 1450 degrees C). In this study, the amount and rate of CO2 uptake by air lime-based materials are quantitatively evaluated under ambient curing conditions of 20 degrees C, 60% relative humidity, and 0.04% CO2 concentration. In addition, the effects of the water-to-binder ratio (w/b) and silica fume addition on the material properties of the air lime mortar, such as strength, weight change, carbonation depth, and pore structure, are investigated. Unlike hydraulic materials, such as Portland cement, the air lime mortar did not set and harden under a sealed curing condition, however, once exposed to dry air, the mortar began to harden by absorbing CO2. During the first week, most of the internal water evaporated, thus, the mortar weight was greatly reduced. After that, however, both the weight and the compressive strength consistently increased for at least 180 days due to the carbonation reaction. Based on the 91-day properties, replacing 10% of hydrated lime with silica fume improved the compressive and flexural strengths by 27% and 13% respectively, whereas increasing the w/b from 0.4 to 0.6 decreased both strengths by 29% due to the increased volume of the capillary pores. The addition of silica fume and the change in the w/b had no significant impact on the amount of CO2 uptake, but these two factors were effective in accelerating the CO2 uptake rate before 28 days. Lastly, the air lime-based material was evaluated to be capable of recovering half of the emitted CO2 during the manufacture of hydrated lime within 3 months.