The effects of the water–binder ratio and different graphene oxide (GO) sizes on the mechanical properties of GO-cement composites were systematically studied by preparing GO-cement mortars. The scanning electron microscopy observation (SEM) of the surface and fracture surface of cement pastes was carried out to study the morphology of cement hydration crystals in GO-cement systems under different space conditions. It was found that GO nanosheets significantly improved the compressive, flexural, and tensile strengths of cement mortars. When the dosage of GO nanosheets was 0.03% by weight of cement, the compressive, flexural, and tensile strengths at 28 days increased by 21.37%, 39.62%, and 53.77%, respectively, but GO was not found to be able to regulate the formation of flower-like cement hydration crystals. It was only shown that the growth space had an important influence on the morphology of hydrates. A possible working mechanism was proposed by which GO nanosheets prevented the expansion of microcracks in the cement pastes via a shield effect, thus enhancing the strength and toughness of the cement composites.