The relationship between the magnetorheology of bimodal magnetic elastomers with high concentrations (60 vol %) of plastic beads with diameters of 8 or 200 μm and the meso-structure of the particles was investigated. Dynamic viscoelasticity measurements revealed that the change in storage modulus of the bimodal elastomer with 200 μm beads was 2.8 × 105 Pa at a magnetic field of 370 mT. The change in the storage modulus for monomodal elastomer without beads was 4.9 × 104 Pa. The bimodal elastomer with 8 μm beads hardly responded to the magnetic field. In-situ observation for the particle morphology was performed using synchrotron X-ray CT. For the bimodal elastomer with 200 μm beads, a highly aligned structure of magnetic particles was observed in the gaps between the beads when the magnetic field was applied. On the other hand, for the bimodal elastomer with 8 μm beads, no chain structure of magnetic particles was observed. The orientation angle between the long axis of the aggregation of magnetic particles and the magnetic field direction was determined by an image analysis in three dimensions. The orientation angle varied from 56° to 11° for the bimodal elastomer with 200 μm beads and from 64° to 49° for that with 8 μm beads by applying the magnetic field. The orientation angle of the monomodal elastomer without beads changed from 63° to 21°. It was found that the addition of beads with a diameter of 200 μm linked the chains of magnetic particles, while beads with a diameter of 8 μm prevented the chain formation of the magnetic particles.