Dielectric elastomers are highly deformable and fast response smart materials capable of actuation under electric fields. Among commercially available dielectric elastomers, silicone rubber can be compounded with different fillers in order to modify its electrical and mechanical properties. To study the effect of organically modified montmorillonite (OMMT) on the dielectric properties of silicone rubber, OMMT was added to this rubber at two levels, 2% and 5%, using two methods, low-shear and high-shear mixing. Composites were characterized by x-ray diffraction (XRD), scanning electron microscopy (SEM), and atomic force microscopy (AFM). The XRD patterns showed different crystallite structures for silicate platelets in the rubber matrix as a result of the two different mixing methods. In low-shear mixing, the ordered crystallite structure of the clay remains almost unchanged, whereas in high-shear mixing it loses its ordered structure, leading to the disappearance of the diffraction peaks. SEM and AFM micrographs depicted better dispersion and more uniform distribution of the organo-clay under high-shear mixing compared to those obtained by low-shear mixing. The tensile properties also confirmed the different degree of dispersion of the nano-clay resulting from the two different methods of mixing. The dielectric properties of the composites were measured under AC electric fields, and the results were compared with reference silicone rubbers with no OMMT. It was shown that the order of organo-clay layers in the less dispersed structure of the clay imparts an additional ionic polarization and higher dielectric permittivity compared to the case where the clay layers are more dispersed and lost their order. The storage and loss dielectric constants of base silicone rubber increase when it is compounded with OMMT.