Magnetorheological elastomers (MREs), a class of polymer-based composites with dispersed ferromagnetic micro-particles, fall in the class of smart materials, because their macroscopic or effective rheological properties can be continuously, rapidly, and reversibly changed with the application of a magnetic field. Conventional magnetorheological elastomers exhibit poor mechanical properties and magnetorheological effect as a result of their matrix materials and the particle-matrix interfaces. Here, we investigate the effect of acetone contents on the magnetorheological elastomer microstructure at the interfacial regions using the scanning electron microscope and the three-dimensional nano-CT imaging, as well as determining the overall or effective mechanical properties of magnetorheological elastomers. It is shown that acetone increases both the overall storage modulus and loss factor along with the magnetorheological effect due to acetone’s reaction on the interface as well as its effect on iron particle alignment.