Due to some useful mechanical, dynamic, and dielectric properties along with the ease of processing and forming, liquid rubbers are ideal materials for fabricating dielectric elastomer actuators in various configurations and for many potential applications ranging from automation to automobile and medical industry. In this study, we present a cross-linkable liquid rubber composition where amine-catalyzed esterification reactions lead to the formation of a network structure based on anhydride functional isoprene rubber, carboxyl-terminated nitrile-butadiene rubber, and epoxy end-capped prepolymers. The success of this intricate network formation procedure was verified by HR-MAS NMR spectroscopy. The new isoprene-based elastomeric material exhibits actuation-relevant attributes including a low elastic modulus of 0.45 MPa, soft response to an applied load up to a large deformation of 300%, and a dielectric constant value (2.6) higher than the conventional Elastosil silicone (2.2). A dot actuator comprising of an isoprene dielectric elastomer film in unstretched state and carbon paste electrodes was fabricated that demonstrated an electrode deformation of 0.63%, which is nearly twice as high as for the commercial Elastosil 2030 film (∼0.30%) at 5 kV. Compared to the Elastosil silicone film, the enhanced performance is attributed to the low modulus and high dielectric constant value of the new isoprene elastomer.