The pozzolanic activity of nano-SiO2 and silica fume was comparatively studied by X-ray diffraction (XRD), differential scanning calorimetry (DSC), scanning electron microscopy (SEM) and the compressive, bond and bending strengths of hardened paste and concrete were also measured. Results indicate that the compressive strength development of the paste made from Ca(OH)2 and nano-SiO2, the reaction rate of Ca(OH)2 with nano-SiO2 and the velocity of C-S-H gel formation from Ca(OH)2 with nano-SiO2 showed marked increases over those of Ca(OH)2 with silica fume. Furthermore, the bond strength at the interface between aggregate and hardened cement paste, and the bending strength of concrete incorporated with 3% NS increased more than those with SF, especially at early ages. To sum up, the pozzolanic activity of nano-SiO2 was much greater than that of silica fume. The results suggest that with a small amount of nano-SiO2,the Ca(OH)2 crystal at the interface between hardened cement paste and aggregate at early ages may be effectively absorbed in high performance concrete.