Research on cement-based materials is trying to exploit the synergies that nanomaterials can provide. This paper describes the findings reported in the last decade on the improvement of these materials regarding, on the one hand, their mechanical performance and, on the other hand, the new properties they provide. These features are mainly based on the electrical and chemical characteristics of nanomaterials, thus allowing cement-based elements to acquire “smart” functions. In this paper, we provide a quantitative approach to the reinforcements achieved to date. The fundamental concepts of nanoscience are introduced and the need of both sophisticated devices to identify nanostructures and techniques to disperse nanomaterials in the cement paste are also highlighted. Promising results have been obtained, but, in order to turn these advances into commercial products, technical, social and standardisation barriers should be overcome. From the results collected, it can be deduced that nanomaterials are able to reduce the consumption of cement because of their reinforcing effect, as well as to convert cement-based products into electric/thermal sensors or crack repairing materials. The main obstacle to foster the implementation of such applications worldwide is the high cost of their synthesis and dispersion techniques, especially for carbon nanotubes and graphene oxide.