The grouting technique is an important method in underground engineering that prevents water seepage and reinforces fractured rock mass. In this research, ultrafine cement-based grouting material, including ultrafine cement (UC), ultrafine fly ash (UFA), polycarboxylate superplasticizer (SP), colloidal nanosilica (CNS), sodium sulfate solution (SS) and water, was developed. The flow time, viscosity, bleeding, setting time and uniaxial compressive strength of the UC-based slurry were measured by orthogonal experiments, and the optimal mix proportion of the UC-based slurry was obtained based on the Taguchi-Grey relational analysis method. Microstructure analysis of the UC-based slurry was conducted using scanning electron microscopy (SEM) and mercury intrusion porosimetry (MIP) tests. The results showed that the Bingham model could provide a satisfactory description of the rheological properties of the UC-based slurry. The addition of CNS and SS could promote the hydration of the UC-based slurry and improve the microstructure of the hardened slurry, thereby increasing the strength of the hardened slurry. The optimum ratio for the UC-based slurry was water/solid (W/S) ratio of 1.0, and the contents of UFA, SP, CNS and SS by mass of UC were 40%, 0.2%, 4% and 4%, respectively.