This paper studied the effect of nano-CaCO3 on workability, strength development, and pore structures of cement paste and self-consolidating concrete. The effects of dosage and size of nano-CaCO3 were considered. For the workability, slump flow (total spread and T50 time), L-box, and V-funnel tests were conducted. The compressive strength was tested at 1, 7, and 28 days for concrete and 1 and 7 days for cement paste. The pore structure, including pore size distribution and volume, was measured using nitrogen adsorption method. The results show that the addition of nano-CaCO3 reduced the setting times. Concrete with a low content of nano-CaCO3 (≤2.5%) had satisfactory workability. No segregation was observed for all concrete specimens. The addition of nano-CaCO3 increased the compressive strength of the concrete and paste. The compressive strength decreased as the particle size increased. The addition of nano-CaCO3 reduced the average pore diameter. XRD test showed no new hydration products.