Despite their excellent performance, two-dimension nanomaterials have certain limitations in improving the performance of cement-based materials due to their poor dispersity in the alkaline environment. This paper has synthesized a new two-dimension stacked GO-SiO2 (GOS) hybrid through the sol-gel method. Nano-SiO2 is coated on the surface of GO with wrinkling characteristics, and the atomic ratio of C, O, and Si in GOS is 1:1.69:0.57. The paper discusses the impacts on the spreading, Marsh cone flow time, rheological properties, mechanical properties, and microstructure of cement-based materials for the GOS at different mixing quantities. Furthermore, with the same mixing quantity of 0.01%, the influences on the dispersity, flow properties, rheological parameters, and mechanical properties of GOS and graphene oxide (GO) are compared. Lastly, fuzzy matrix analysis has been adopted to analyze the comprehensive performance of cement-based materials containing GOS. The research results indicate that, compared with the reference sample, the spreading for the GOS cement mortar with 0.01% mixing quantity was reduced by 4.76%, the yield shear stress increased by 37.43%, and the equivalent plastic viscosity was elevated by 2.62%. In terms of the 28 d cement pastes, the compressive and flexural strength were boosted by 27.17% and 42.86%, respectively. According to the optical observation, GOS shows better dispersion stability in the saturated calcium hydroxide solution and simulated pore solution than GO. Compared with the cement-based materials with the same mixing quantity (0.01%), GOS has higher spreading, lower shear yield stress, and higher compressive and flexural strength than GO. Finally, according to the results of fuzzy matrix analysis, when the concentration of GOS is 0.01%, it presents a more excellent comprehensive performance with the highest score. Among the performance indicators, the most significant improvement was in the flexural properties of cement-based materials, which increased from 8.6 MPa to 12.3 MPa on the 28 d.