In this work, a kind of ternary hybrid material, MIL-125/MoS2/SiO2, was prepared by a solvothermal and Stöber method. In this system, MIL-125, as the matrix material, not only furnishes a large specific surface area for MIL-125/MoS2/SiO2, thereby providing a basis for stronger interfacial polarization, but also effectively enhances the antisettlement ability of the electrorheological fluids (ERFs). Different characterizations, such as scanning electron microscopy, transmission electron microscopy, XRD, XPS, FT-IR, BET, electron mapping, etc., were used to analyze the ternary nanohybrid. The ERFs prepared by combining the different advantages of the three materials in the hybrid system were studied by a HAAKE high-speed rotary rheometer. In addition, the combination of MoS2 and SiO2 provides suitable electrical conductivity and dielectric properties for the system to promote the generation of interface polarization, ensuring that the entire system exhibits stronger electrorheological behavior without electrical breakdown and thus obtains higher shear stress.