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Networks of conductive nanoparticles have been used as electrodes for dielectric elastomer actuator multilayers because of their excellent extensibility and low added stiffness. Nanoparticle network topography, however, has typically effected a tradeoff between conductivity and breakdown strength. This has limited actuators to a corresponding tradeoff between either high operating frequencies and efficiencies or high stresses, strains, and energy densities. This tradeoff is resolved by spatially patterning multiple nanoparticles to produce hybrid electrodes. Sparse networks of high‐aspect‐ratio carbon nanotubes allow for self‐clearing in the body of the electrode, yielding 54.7 V µm−1 breakdown strength, 86.4% that of the neat elastomer. Dense networks of low‐aspect‐ratio carbon black at the external interfaces, meanwhile, provide low contact resistance (44.09 kΩmm). Two tools essential for their practical deployment are developed: a scalable fabrication process and an automated pre‐clearing algorithm. The fabrication method leverages the batch spray and stamp paradigm in concert with vacuum filtration to scalably deposit nanoparticle electrodes with minimal parameter tuning, enabling the production of a 100‐layer actuator capable of 14% strain. The adaptive pre‐clearing algorithm discriminates between and responds to a range of defect‐induced failures in newly fabricated actuators, eliminating the need for human oversight and standardizing the break‐in procedure. [ABSTRACT FROM AUTHOR]

Multilayer dielectric elastomer actuators have a wide range of potential applications, but their development and commercial implementation have been hindered by existing manufacturing processes. Existing processes are low‐throughput, limited in area, and/or can only process a narrow range of elastomers. This study presents a novel fabrication paradigm that overcomes these challenges: instead of sequentially patterning electrodes directly onto successive elastomer layers, electrode stamps are patterned onto a carrier film in an independent batch‐spray process and the electrodes are then stamp‐transferred onto each elastomer layer. By modularizing the production and assembly of electrodes, a laboratory‐scale implementation of the process achieves a throughput of 15 layers h−1, a maximum electrode size of 300×300 mm, and tuning‐free compatibility with a wide range of elastomers. The batch‐spraying paradigm also provides the unique capability to evaluate and modify electrodes before they are assembled into a multilayer; a method of mechanically treating the electrodes is employed to increase the breakdown strength of Elastosil P7670 devices from 15.7 to 33.5 V µm−1. The electrodes are conductive up to a strain of more than 200% and add negligible stiffness to the multilayer structure. The capabilities of this process to produce useful devices are demonstrated with a large‐area loudspeaker and an actuator with 60 active layers. [ABSTRACT FROM AUTHOR]