Abstract Carbon-black nanoparticles (CBN) have been incorporated into cement-based materials for improvement of mechanical or self-sensing properties. There is no previous research focused on the microstructural evaluation of effects of CBN on both parameters. In this work, mortars containing different CBN contents were produced, cured for 28 days, and subjected to electron microscopy (SEM), X-ray diffraction (XRD) and Raman spectroscopy. Tests for determination of compressive strength, modulus of elasticity and piezoresistivity response were developed. SEM indicated that lower CBN contents refined the cementitious matrix, while higher contents increased the volume of voids. XRD and Raman spectroscopy indicated hydration improvements for CBN contents between 0.375% and 3%. The best mechanical improvements were provided by concentrations of CBN up to 3%. CBN contents of 5% and 6% provided the best sensing properties. The optimal concentration was found to be 5% of CBN, since it provided excellent piezoresistivity, without significant mechanical properties loss.