This study investigates the hydrothermal synthesis of calcium silicate hydrate (C-S-H) seeds using nano-size glass powder (NGP) derived from siliceous raw materials and CaO as the calcareous precursor. The influence of varying NGP concentrations on the particle size, microstructure, and phase composition of the C-S-H seeds was systematically analyzed. The synthesized C-S-H seeds were subsequently employed as additives to evaluate their effects on the early hydration process and compressive strength development of cement paste. The results indicate that increasing the NGP concentration from 0.2 mol/L to 0.8 mol/L leads to an exponential increase in the median particle size of the C-S-H seeds from 147 nm to 1328 nm and a corresponding morphological transformation from flocculent to granular structures. Additionally, the purity of the C-S-H sample decreased from 74.8% to 54.5% as the NGP concentration increased. The addition of C-S-H seeds can increase the 12h compressive strength of cement pastes by 15.5%–53.5%. This improvement is due to the accelerated early hydration kinetics induced by the C-S-H seeds, which act as nucleation sites, thereby increasing the nucleation and growth rates by 31.4% and 53.2%, respectively.