The carbonation technique was applied to accelerate the hydration of low heat portland cement (LHC). Before carbonation, the demoulded pastes were precured in water for 0, 2, 7, and 21 d, respectively. The results show that procuring time in water strongly influences the carbonation process. The phenolphthalein test indicates that the paste precured in water for a shorter time is more quickly carbonated than that for a longer time. The content of calcium hydroxide increases with increasing the procuring time in water, whereas, the amount of absorbed carbon dioxide changes contrarily. Scanning electron microscope (SEM) observation shows that portlandite always fills up big air bubbles in the paste during precuring in water, and the mercury intrusion porosimetry (MIP) results show that there are less large capillary pores in the paste precured in water for a longer time. It is found that the paste without precuring in water has more carbon dioxide absorption during curing in carbon dioxide atmosphere, and its total pore volume decreases remarkably with an increase in the carbonation time than that precured in water. X-ray diffraction (XRD) and Brunauer-Emmett-Teller (BET) surface area analyses indicate that the carbonate products are vaterite and calcite; CxSHy,, formed from carbonation has low BET surface area in comparison with that of C-S-H formed from curing in water.