Cement production is responsible for 5% of CO2 emissions worldwide. The concern about the pollution derived from the construction industry has brought attention to the need of developing more sustainable construction materials and processes. Admixtures based on nanometric graphene oxide have the potential to enhance mechanical properties and durability of cementitious composites. In this context, an experimental program was conducted to evaluate how the addition of graphene oxide may be used to reduce cement content in concretes, maintaining the same mechanical properties of conventional concretes (control matrices, with no graphene oxide additions). Kinetics of hydration of cement pastes was evaluated by isothermal calorimetry, phase evolution during hydration was determined by X-ray diffraction coupled with quantitative Rietveld analysis and mechanical properties were evaluated by compressive strength. Results indicate that graphene oxide additions provide a faster hydration rate until 24 h and generate a larger amount of C-S-H gel, increasing mechanical strength of the matrix. By the addition of graphene oxide dispersion (0.4% of solid content) at 0.02% by cement weight, cement content reductions of up to 15% may be achieved, maintaining the same compressive strength as the control matrices. From this research, a reduction in cement content to obtain more sustainable construction materials and processes may be achieved.