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Magnetoactive elastomers (MAE) based on soft silicone matrices, filled with various proportions of large diameter (approximately 50 μm) iron and small diameter (approximately 0.5 μm) magnetite particles are synthesized. Their rheological behavior in homogeneous magnetic fields up to 600 mT is studied in detail. The addition of small magnetite particles facilitates fabrication of uniformly distributed magnetic elastomer composites by preventing aggregation and sedimentation of large particles during curing. It is shown that using the proposed bimodal filler particles it is possible to tailor various magnetorheological (MR) properties which can be useful for different target applications. In particular, either absolute or relative magnetorheological effects can be tuned. The value of the damping factor as well as the range of deformation amplitudes for the linear viscoelastic regime can be chosen. The interdependencies between different MR properties of bimodal MAEs are considered. The results are discussed in the model framework of particle network formation under the simultaneous influence of external magnetic fields and mechanical deformation. [ABSTRACT FROM AUTHOR]