The paper tests the influence of mass fractions of carbonyl iron particles (CIPs) on the rheological properties of magnetorheological (MR) gels. Polyurethane-based MR gels with different weight fraction of CIPs, i.e., 40, 60, and 80%, were firstly prepared by mechanical mixing, respectively. The changes of shear stress and viscosity with shear rate under different magnetic flux density were tested and analyzed. It was found that the shear stress increases with mass fraction under magnetic flux density. The viscoelastic properties of MRGs were achieved by oscillatory shear measure. The effects of strain amplitude and frequency on viscoelastic of MRGs under different magnetic flux density were measured and analyzed. The study results shown that the elastic characteristics become more obvious with the increase of CIPs mass fraction. However, it has opposite effect on the viscous properties of materials.