This paper develops a kind of molded disc samples to investigate the carbonation and related behaviors of hardened cement pastes under different previous hydration degrees. Weight and length changes of cement pastes over time are monitored during a multistep process including carbonation, drying, rewetting, and redrying. The combination of X-ray diffraction (XRD) and thermogravimetric analysis (TGA) is used to identify and quantify the mineral compositions of carbonated cement pastes. An exponential function between CO₂ uptake capacity and hydration time of cement pastes is established, which shows that the CO₂ uptake capacity of cement pastes decreases dramatically at the very beginning days of hydration and then remaining relatively stable as hydration time is prolonged. Two reasons for this finding are revealed: i) the equilibrium between the carbonation and the post-carbonation reaction of carbonation product, i.e., silica-alumina gel; ii) refining of pore structures by hydration products which hinders carbonation. A clearer zonation of carbonation areas is proposed, and the spatial distribution equations of CO₂ absorption are initially established. By monitoring carbonation and drying behavior of cement pastes with different hydration ages, it is revealed that carbonation reduces drying shrinkage of cement pastes especially for early-age samples, whereas drying increases carbonation shrinkage. By investigating the water changes during the multistep process, it is found that water is little released during the carbonation of C–S–H gels. New insight into mechanism of carbonation shrinkage is provided by a newly proposed model.