Magnetorheological (MR) elastomers, which are mainly composed of magnetic particles and elastic polymer, are a new kind of smart materials whose modulus can be controlled by changing the strength of magnetic fields. In this article, MR elastomers based on immiscible silicon rubber/polystyrene (SR/PS) blend matrix were fabricated successfully via cosolvent method and the MR effect, electric and mechanical properties, and the microstructures of the corresponding materials were studied. SEM studies showed that the dispersion of iron particles in blend matrix were different from that in single polymer, which could be further proved by the different electric conductivity. The MR effect of MR elastomers based on blend matrix varied with the different ratios of SR and PS, which was discussed in detail from the special dispersion of iron particles and of zero-modulus of MR elastomers. In addition, the MR elastomers based on SR/PS blend matrix had enhanced mechanical properties, which made them more hopeful to be applied in practice.