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Dielectric elastomer actuators (DEAs) are promising soft electromechanical transducers for soft robotics. Fabricating a high‐performance DEA actuated by sub‐kV voltage remains challenging. Here, a facile method not only to fabricate ultrathin dielectric elastomer films of triblock copolymers but also to enhance the dielectric breakdown strength and thus enhance the electromechanical performance is reported. A thick thermoplastic elastomer film of poly(styrene‐b‐butyl acrylate‐b‐styrene) from solution blading is symmetrically pre‐stretched and relaxed at 120 °C to fabricate a freestanding ultrathin DE film. Compared with the pristine DE film of the same thickness (12 µm), the thermally‐relaxed DE film with equally biaxial pre‐stretch ratio 3.5 × 3.5 exhibits increased electrical breakdown strength by a factor of 1.9 (from 43 to 82 V µm⁻¹), maximum actuation area strain by a factor of 1.9 (from 11.7% to 22.4%), and …