In this paper, we investigate the CO2 carbonation on porous materials such as the cement paste mortar. Our scientific goal is to model the CO2 carbonation effect on the porous cement mortar by the micro-dilatation theory and to determine the chemo-mechanical stress development due to the chemical reactions. In fact, this phenomenon will modify not only the pH value of the cement paste but also the micro-structure due to collapsing pore-network. Based upon the micro-dilatation theory originally proposed by Cowin and Nunziato, four unknown parameters related to the micro-structure will be determined for the cement mortar using the semi-empirical method and numerical modeling. The experimental carbonation tests on two different types of cement paste (CEMI and CEMIII) have been realized to capture carbonated affected zones and to measure their shrinkage deformations.