This is the first review that presents an outlook on sol-gel science’s potential in different areas of cement science and chemistry. Progress in nanotechnology has shown sol-gel science possibilities to advance knowledge and modify the C-S-H structure at the nanolevel. There is a longstanding work in several areas of cement and concrete research to understand cement hydration mechanisms and to study the structure of C-S-H. Researchers have made attempts to tailor C-S-H through the addition of silanes, which has aided understanding of its structure. Research on sol-gel science in various fields of cement science has been increasing recently because of promising results. Overall it is shown that a change in sol-gel parameters has a significant impact on cement hydration. This review indicates how sol-gel technology can be further exploited to investigate and improve the hydrated cement microstructure.