Magnetorheological fluids (MRFs) are primarily composed of magnetic particles suspended in carrier liquids, exhibiting a remarkable capacity to respond dynamically to external magnetic fields. However, the phenomenon of solid–liquid phase separation, attributable to particle sedimentation, represents a formidable barrier to the real-world application of MRFs in engineering contexts. As a result, it becomes critically imperative to conduct a thorough investigation into the sedimentation behavior of MRFs under static conditions, to significantly enhance their practical utility. In the study, computational analysis through COMSOL was utilized to elucidate the sedimentation dynamics of MRFs. The findings indicated that particle sedimentation harbored the potential to induce localized turbulence within the flow field, thereby significantly impacting the sedimentation dynamics of MRFs. The motion of particles consistently followed a pattern where sedimentation rates decreased as the viscosity of the carrier liquids increased. Moreover, the elucidation of the settling behavior of MRFs was facilitated by the introduction of two dimensionless numbers. These dimensionless numbers were employed to systematically characterize the temporal evolution of the supernatant height throughout the settling process. This investigation further explored the intricate interdependence between these dimensionless parameters via a comprehensive series of settling experiments. The outcomes of this research uncovered a unique pattern in the solid–liquid separation process of MRFs, marked by a phase of gradual initiation, followed by acceleration, and culminating in deceleration. However, as the viscosity of the carrier liquids increased, this pattern became less pronounced, gradually shifting toward a more uniform settling trajectory.