To exploretheeffects of physical, mechanical, anti-deterioration properties of graphene oxide (GO) on cement-based cementitious materials, GO sheet dispersions areprepared by the improved Hummers method and ultrasonic dispersion method. The influence of theGO content on the compressive and flexural strengths of cement paste is investigated, and the penetration process of chloride ions in graphene oxide concrete is discussed by the electric accelerated erosion method. Combined with the rapid freeze-thaw test, the deterioration of graphene oxide concrete ismethodically analyzed. Theobtained results reveal that an appropriate amount of GO improves both the compressive and flexural strengths of cement pastev. In the chloride environment, the chloride diffusion coefficient of 0.03% GO concrete is 18.75% less than that of ordinary concrete.Under the action of freeze-thaw cycles, with the increase of salt freezing times, the deterioration mode of GO concrete is a combination of mortar shedding, micro-crack expansion, denudation, and block shedding; The stress-strain curve of the specimen tends to be flat with the growth of salt freezing times. The peak stress gradually lessens, the peak strain gradually grows, and the elastic modulus remarkably reduces. Compared with ordinary cement paste, theGO is capable of promoting the growth of cement paste hydration crystals, changing the size and shape of crystals, and realizingthe regulation of cement paste microstructure. Incorporating an appropriate amount of theGO could promote the cement hydration process and enhance the chemical water-binding amount in the cement paste. The optimal GO content is reported to be 0.03% of the cement mass.