AbstractDielectric elastomer actuators (DEAs) face an acknowledged challenge: On the one hand, the majority of elastomers only achieve small electroactive deformation (<20%) in the absence of prestretch; on the other hand, rare elastomers capable of showing large electroactive deformation require relatively complicated processing and chemistry. This work addresses this challenge by fabricating an elastomer with a network of large side groups, which achieves a very large electroactive deformation (218%) without pre‐stretch. This elastomer can be rapidly and massively fabricated within a few min, by polymerizing a commercial monomer with a large alkyl side group. The large side groups in the polymer network repel each other and extend the load‐bearing strands, which results in a pronounced strain‐hardening behavior. This behavior helps the elastomer to get rid of electromechanical instability during actuation and hence to exhibit a large electro‐active deformation, a high energy density (>> human muscle), and a large output force (≈500 times self‐weight). the elastomer capable of manufacturing a soft electroactive gripper is demonstrated with large deformation, large force, and rapid response, which enables grasping fragile objects of various complex shapes in an agile away.