Ground granulated blast-furnace slag (GGBS), a waste product generated during steel production, can be added as a substitute for cement in concrete to mitigate the environmental impact of the cement and steel industries. However, the use of GGBS is limited because it decreases the early strength development of cement or concrete. This study evaluated the performance of incorporating synthesized C-S-H nanoparticles to enhance the compressive strength, early hydration, and microstructure of cement composite. The synthesized C-S-H nanoparticles were produced at standard atmospheric pressure and room temperature. Heat of hydration, X-ray diffraction, and thermogravimetric analyses were conducted to investigate the hydration and mechanical properties of the cement containing the C-S-H nanoparticles. Further, mercury intrusion porosimetry was conducted to examine the pore structures. The experimental finding demonstrated that adding C-S-H nanoparticles accelerated the early hydration progress in the cement composites, thereby increasing their initial compressive strength.