In this work, nanofibers and cellulose nanocrystals from the native Amazonian bamboo Guadua weberbabeuri were used in structural cementitious composites. Through the preparation of bamboo nanofibers—bleached cellulose pulp (BCP) and cellulose nanocrystals (CNC), as well as obtaining shredded bamboo (SB) and delignified cellulose pulp (DCP)— the additions corresponding to the additive nanomaterials were characterized with physical tests such as water absorption, specific mass, void index, and dimensional variation. A mechanical tensile strength test was carried out at 28 days, with an incorporation content of 0.40% of mass in relation to the cement. The results indicated, in relation to the control, improvement in the physical properties, especially in the additions with nanofibers and cellulose nanocrystals. For the mechanical tensile strength tests, the indicator allowed an increase of 14.60% with the addition of nanofibers and 12.70% in the addition of nanocrystals. Therefore, with the execution carried out, it could be seen that the incorporation was able to generate optimization in the joint performance of the materials under analysis, reinforcing the practices and ideals arising from civil engineering, nanotechnology, and sustainability.
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