A recent advance in construction technology is the use of self-healing cementitious materials containing synthetic microfibers and superabsorbent polymers. By stimulating autogenous healing by means of superabsorbent polymers, cracks are closed and this will cause an increase in durability and service life. However, this improved healing capacity has not been quantified yet in terms of increased further hydration and volume of healing products. This is needed to model the material and to stimulate the practical application in constructions. This paper provides quantitative data, obtained by an NMR study. Addition of 1 m% of selected superabsorbent polymer versus cement to a cementitious material, stimulated further hydration with nearly 40% in comparison with a traditional cementitious material, if 1 h water contact per day was allowed. At 90% relative humidity, no healing was observed in reference samples. While the further hydration around a crack in specimens with superabsorbent polymers was still 68% of that of a reference system with cyclic water contact, due to the uptake of moisture by the superabsorbent polymers. As such, NMR results quantify the positive influence of superabsorbent polymers in terms of stimulated autogenous healing and substantiate their benefits for application in the construction area.