Soft robots are intrinsically safe for use near humans and adaptable when operated in unstructured environments, thereby offering capabilities beyond traditional robots based on rigid components. Soft actuators are key components of soft robots; recently developed hydraulically amplified self‐healing electrostatic (HASEL) actuators provide a versatile framework to create high‐speed actuators with excellent all‐around performance. Peano‐HASEL actuators linearly contract upon application of voltage, closely mimicking the behavior of muscle. Peano‐HASEL actuators, however, produce a maximum strain of ≈15%, while skeletal muscles achieve ≈20% on average. Here, a new type of HASEL is introduced, termed high‐strain Peano‐HASEL (HS‐Peano‐HASEL) actuator, that achieves linear contraction up to ≈24%. A wide range of performance metrics are investigated, and the maximum strain of multiunit HS‐Peano‐HASEL actuators is optimized by varying materials and geometry. Furthermore, an artificial circular muscle (ACM) based on the HS‐Peano‐HASEL acts as a tubular pump, resembling the primordial heart of an ascidian. Additionally, a strain‐amplifying pulley system is introduced to increase the maximum strain of an HS‐Peano‐HASEL to 42%. The muscle‐like maximum actuation strain and excellent demonstrated all‐around performance of HS‐Peano‐HASEL actuators make them promising candidates for use in artificial organs, life‐like robotic faces, and a variety of other robotic systems.

Combating environmental pollution demands a focus on sustainability, in particular from rapidly advancing technologies that are poised to be ubiquitous in modern societies. Among these, soft robotics promises to replace conventional rigid machines for applications requiring adaptability and dexterity. For key components of soft robots, such as soft actuators, it is thus important to explore sustainable options like bioderived and biodegradable materials. We introduce systematically determined compatible materials systems for the creation of fully biodegradable, high-performance electrohydraulic soft actuators, based on various biodegradable polymer films, ester-based liquid dielectric, and NaCl-infused gelatin hydrogel. We demonstrate that these biodegradable actuators reliably operate up to high electric fields of 200 V/μm, show performance comparable to nonbiodegradable counterparts, and survive more than 100,000 actuation cycles. Furthermore, we build a robotic gripper based on biodegradable soft actuators that is readily compatible with commercial robot arms, encouraging wider use of biodegradable materials systems in soft robotics.

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