Durability of concrete exposed to an external sulfate attack is a great concern for the long-term reliability of nuclear waste containment. This paper presents experimental results obtained on cement paste subjected to a low concentration (30 ×10−3 mol/L) external sulfate attack. Samples were characterized with complementary methods (XRD, SEM-EDS, microtomography, microindentation, autoradiography) to follow the evolution of chemical, mineralogical, microstructural and mechanical properties during 8 months. Cement pastes of different C3A contents were used to boost either ettringite or gypsum formation during the sulfate attack to assess their respective impact on the degradation. Cracks parallel to the attacked surface occurred in the zone of gypsum formation and portlandite dissolution, which suggests that gypsum has a key effect on the expansion. Reactive transport modeling supported the discussion on the competition between hydrolysis, gypsum and ettringite precipitation as well as the analytical homogenization to estimate Young’s moduli.