This work aims at evaluating the influence of curing conditions on the carbonation process of lime-based mortars and pastes and on the resulting mineralogical, macro- and microstructural properties. To this end, lime-based materials (mortars and pastes) were subjected to natural (0.05 % CO2) and accelerated (5 % CO2) carbonation. The influence of factors such as water/binder ratio, lime (agglomerated) particle size (surface area) and presence of admixtures on the carbonation process was also addressed. The materials cured under the CO2-rich atmosphere carbonated faster and reached a higher degree of carbonation after only 7 days than those cured naturally for 3 years, even though total carbonation was not achieved. Nevertheless, due to the high conversion rate, the evolution of the properties of the tested materials after being subjected to accelerated carbonation for 7 days is expected to be minimal (stable properties were reached). Portlandite was mostly converted into calcite that precipitated as rhombohedral and scalenohedral crystals regardless of the curing environment. The crystals appeared to be larger and better developed in the specimens subjected to accelerated carbonation, which contributed to the higher mechanical strength displayed by these mortars.