The geoenergy industry has challenging demands on cements used as downhole materials. Once placed in the annular space, the cement sheath must be very low permeability and mechanically durable. Its characteristics are strongly influenced by its microstructure. A holistic approach, including combined mineralogical, physical, and mechanical investigations, provides a better understanding of how these characteristics interplay. Class G cement was investigated and compared to cement formulations containing carbon black or silica fu me, trying to tailor its performance. The addition of carbon black and silica fume has some effect on the modal and chemical phase composition and results in a much denser microstructure. Furthermore, porosity is reduced while the pore size distribution remains similar. Samples containing carbon black have a reduced Young’s modulus, indicating a more plastic behavior. The addition of silica fume increased both mechanical strength and permeability. However, comparable results can also be achieved by carefully tuning the water/cement ratio of the initial slurry.