Carbonation of hydrated cement paste (HCP) under γ-irradiation is researched in this paper. It is supposed that radiation-induced carbonation takes part simultaneously with “natural” carbonation. “Natural” carbonation is governed by diffusion and therefore takes part in the material close to surface only, whereas radiation-induced carbonation manifests in all irradiated material. The hypothesis has been tested by means of three sets of experiments. Within these experiments the following changes were investigated: (a) changes of composition of hydrated cement paste (transformation of portlandite to calcite), (b) changes of porous space [changes of average pore diameter (APD)], (c) changes of mechanical properties (hardness). HCP was analysed in the surface layer as well as in the centre of samples. The results show clearly that radiation at least accelerates carbonation driven by diffusion and support a hypothesis that besides natural carbonation there is also independent carbonation caused by γ-irradiation.