The effect of the use of TiO2 nanoparticles in the production of cementitious composites, worldwide already known, represents an area of interest for the development of materials with self-cleaning capacity; antimicrobial, antibacterial, antifungal properties; and to contribute to the reduction of environmental pollution. This paper aims to analyze the influence that TiO2 nanoparticles have on the cementitious matrix regarding hydrophilicity, this being one of the two main parameters of the self-cleaning mechanism. Experimental tests, conducted by using the indirect method of measuring the surface water absorption, indicated that an addition of 3%-6% (relative to the amount of cement) of TiO2 nanoparticles is effective in terms of increasing the surface hydrophilicity of the cementitious composites. An excess of TiO2 nanoparticles in the composite matrix (10% TiO2 nanoparticles relative to the amount of cement) not only does not improve surface performance in terms of hydrophilicity, but also reduces them. However, in practice on a case-by-case basis, an analysis is required regarding the optimal amount of nanoparticles used as an addition in the mix-design of the cementitious materials that are intended to induce the quality of self-cleaning process, depending on the intended use, climate, degree and duration of sunlight, and so on.