Abstract: In the cement industry, the morphological control of calcium silicate hydrate (C-S-H) and its impact on cement hardening and hydration are important research topics. This study investigated the impact of template agents on C-S-H morphology and structure. By using chemical precipitation, amorphous, spherical, needle-like, and layered C-S-H with the template agents being sodium dodecyl benzene sulfonate (SDBS) and cetyl trimethyl ammonium bromide (CTAB) were prepared. An increase in SDBS concentration resulted in the transformation of the C-S-H morphology from disorderly to spherical, rod-shaped, and vesicular. When CTAB was used, an increased concentration resulted in the transformation of the C-S-H morphology from disorderly to spherical and layered. When the template agent concentration was greater than the critical micelle concentration (CMC), both the C-S-H crystallinity and CMC value decreased. The impact of different C-S-H morphologies on cement performance particularly cement hydration was also evaluated and analyzed. A significant correlation between cement hydration heat and strength was verified. Different microscopic C-S-H morphologies were used to design cement products, allowing the improvement of cement performance to varying degrees. Experimental results would provide an insight into the improvement of the performance of ordinary cement.