In this study, a new type of cement-based healing pellets (CHPs) were proposed to accelerate the healing efficiency of concrete, which was mainly based on the introduced Na2CO3 on promoting the formation of calcium carbonate (CaCO3) in cracks. The effects of Na2CO3 on the characteristics of CHPs were firstly investigated, and then the properties of cement mortar mixed with CHPs were studied quantitatively, including the workability, mechanical properties and healing ability. The results showed that higher dosages of Na2CO3 in CHPs decreased the size range of pellets and reduced the setting time, fluidity and heat of hydration of mortar. Still more, CHPs reduced the early strength of mortar but kept the intensity growth rate stable such that it had nearly no negative effect on the later strength. With the content of CHPs increasing, the strength of mortar showed a decreasing trend, while the pore-filling efficiency and strength healing rate of mortar were further improved. In addition, as a new type of self-healing pellets for concrete based on the “build-in” carbonation, CHPs improved the strength and healing effectiveness of cement mortar. When the dosage of Na2CO3 in CHPs and the content of CHPs in mortar were at 10% and 25%, respectively, mortar obtained highest strength in the later stage and the best healing effect.