Chemical organic admixtures play a significant role in engineering structures. This paper reviews the effects of organic admixtures with different molecular scales and functional groups on the cement hydration process and discusses their roles in the microstructure and properties of cement-based materials. According to the current research, the molecular structure of admixtures determines their adsorption performance on cement, which in turn affects their mechanism of action and durability in cement-based materials. Incorporating organic admixtures can regulate the properties of cement-based materials. Most admixtures can adsorb onto the surface of cement particles and complex with Ca2+ in the liquid phase, thus exhibiting a retarding effect. The hydration products of cement develop more completely, potentially positively impacting the durability of concrete, particularly its impermeability.