Dielectric elastomers (DEs) can act as deformable capacitors that generate mechanical work in response to an electric field. DEs are often based on commercial acrylic and silicone elastomers. Acrylics require prestretching to achieve high actuation strains and lack processing flexibility. Silicones allow for processability and rapid response but produce much lower strains. In this work, a processable, high-performance dielectric elastomer (PHDE) with a bimodal network structure is synthesized, and its electromechanical properties are tailored by adjusting cross-linkers and hydrogen bonding within the elastomer network. The PHDE exhibits a maximum areal strain of 190% and maintains strains higher than 110% at 2 hertz without prestretching. A dry stacking process with high efficiency, scalability, and yield enables multilayer actuators that maintain the high actuation performance of single-layer films.