This chapter discusses the development of a materials science approach with an application to nanotechnology to optimize the processing and micro/nanoscale structure of cement-based materials reinforced with nanosized fibers and carbon nanotubes. The dispersion of multi-walled carbon nanotubes (MWCNTs) and carbon nanofibers (CNFs) for use in cementitious composites and specifically the effect of ultrasonication energy are discussed in detail. The nanomechanical properties of the CNT/ CNF cementitious nanocomposites are examined through nanoindentation experiments. Additionally, the excellent reinforcing ability of both the MWCNTs and CNFs is demonstrated. Finally, the effect of the addition of silica nanoparticles on the degradation by calcium leaching is discussed and explained.