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• Multifunctional properties were induced by the combination of NS and NF. • In NS treatments, up to 90% decrease in permeability against external agents. • Treatments applied could be an alternative to prevent deterioration problems. • The NF with short-chain siloxanes, allows greater resistance to degradation. This study evaluated the multifunctional properties that develop during curing on the surfaces of Portland cement-based mortars from using silicon-based nanoparticles (NS) and functionalized nanoparticles (NF). The durability and hydrophobicity were used as indices to determine the performance. Mortar specimens were manufactured with a water to cement (w/c) ratio of 0.65, and different treatments were applied with combinations of 0.1% NS and NF relative to the weight of the water used for curing. In some cases, treatments were performed for 72 h; in others, two layers were applied. The results indicated that the treatments reduced the carbonation depth and the diffusion of Cl- ions. In addition, the treated specimens demonstrated an increase in resistivity due to reduced pore network connectivity; this is evidence of a reduction in permeability and consequently an increase in durability. Multifunctional properties on the surface were demonstrated to be induced by the combination of NS and NF. [ABSTRACT FROM AUTHOR]