ABSTRACT: The principal phase of hardened Portland cement pastes is calcium silicate hydrate (C-S-H), which influences the physical and mechanical properties of construction materials. In this work, calcium silicate hydrate (C-S-H) was synthesized, with the addition of poly-methacrylic acid with sodium (PMA), for the development of C-S-H/ polymer nanocomposites. Among the polymers available, PMA is indicated in the literature as one of those viable for producing C-S-H/polymer complexes. However, no consensus exists regarding the type of interaction this produces. The resulting compounds were characterized by XRD, FT-IR, TGA, carbon content (CHN), TEM, SEM and elastic modulus and hardness were measured by instrumented indentation. A significant change was verified in the nanomechanical properties of C-S-H with PMA, resulting in reduction in the elastic modulus and hardness. The set of results presented do not confirm the intercalation of PMA in the interlayer space of C-S-H, but presented evidence of the potential for intercalation, since changes in the microstructure clearly occurred.