This article presents the development of a new kind of magnetorheological elastomer blend made with natural rubber, acrylonitrile–butadiene rubber (NR-NBR), and electrolytic iron particles through solution mixing. The compressive stress and elastic modulus of the composites in the isotropic and anisotropic states of the filler were studied. A unique study of the filler distribution and filler orientation mechanism was proposed from the compressive properties and scanning electron microscopy. A strong improvement in the elastic modulus of the NR–NBR blend from isotropic to anisotropic change was achieved as compared with NR and NBR in single-rubber composites. The filler content in the anisotropic magnetorheological elastomers was optimized by measuring the field-dependent elastic modulus in the presence of an externally applied magnetic field. The blend rubber composites showed better sensitivity in the presence of a magnetic field than the NR and NBR composites did. The improvement might be due to the better filler orientation and strong adhesion of filler particles by the NR phase in the blend matrix. The new elastomer blends may have applications in active dampers, vibrational absorption, and automotive bushings.