This modelling study investigated the physicochemical and kinetic controls of the mineralogical evolutions of cementitious materials subject to accelerated atmospheric carbonation. Simulations are based on published experimental results on two samples, a hydrated C3S and a C-S-H paste, carbonated for 1 year at 55 % RH at 3 % CO2. For the C3S paste, reactive transport simulations accurately reproduced the mineralogical observations at different time intervals. However, for the C-S-H paste, in which significant cracks appeared, basis simulations could not reproduce the long-term carbonation extent. 2D simulations suggested that potential preexisting cracks could not fully explain the seemingly increasing carbonation rates. A final simulation using a simplified description of the crack appearance during carbonation gave the most accurate representation of the experimental results (degradation depths, mineralogy evolution). This demonstrates that, to accurately estimate the durability of cementitious materials subject to carbonation under dry conditions, coupled geochemical-mechanical descriptions are required.