Basalt materials (e.g., basalt powder, aggregate, and fiber) are commonly used in cement-based materials. To understand the mechanism of the influence of basalt on the properties of cement-based materials (i.e., fluidity, hydration, and strength), zeta potential tests with different Ca2+ concentrations were carried out using basalt powder (BP). It is found that BP has a weaker absorption for Ca2+ compared to cement and quartz particles, which is directly related to its surface chemical properties. This weak absorption has a significant influence on the rheology and early-age hydration of cement paste. Moreover, the morphology of hydrate on the surface of the material observed by scanning electron microscope (SEM) also shows that the growth of CSH on the surface of BP particles is smaller than that of cement particles, indicating that BP delays the formation of CSH. Rheological tests showed that the reduction of BP’s adsorption of calcium ions weakened the electrostatic repulsion between particles, which led to the reduction of rheological properties. The influence of BP on the strength of cement paste was studied through crack characterization and fracture observation. The results show that the interfacial strength between BP and hydration products is very weak and does not increase with the hydration process, and the chemical reaction of BP is not obvious. In addition, the substitution of BP for cement leads to a dilution effect. These factors cause the strength of cement paste to decrease.