Evaluating the effects of nanomaterials in cementitious systems is paramount to projecting high-performance construction materials. However, the synthesis of some nanomaterials on a large scale and their toxicity may limit their application. In this context, nanofibrillated cellulose (NFC), a biodegradable and natural material stand out. Thus, this paper aims to study the influence of NFC on the fresh, hardened properties (compressive and flexural strengths) and mineralogy of cementitious systems. The results indicated that incorporating up 0.075 wt.% to CNF reduced the spread of cement pastes by up to 14.0%. A CNF content of 0.025 wt.% increased the 28-d compressive and flexural strengths by 22.0% and 25.0%, respectively, compared to the control sample. The X-ray diffraction (XRD) results indicate that higher NFC contents (>0.025 wt.%) resulted in lower intensity portlandite peaks after 7 days, which may show a lower hydration degree, especially concerning the plain cement paste. These results suggest that the NFC can affect the hydration of cementitious matrices at early ages; however, it did not significantly affect the hydration degree after 28 days of hydration.