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Constructing soft robotics with safe human-machine interactions requires low-modulus, high-power-density artificial muscles that are sensitive to gentle stimuli. In addition, the ability to resist crack propagation during long-term actuation cycles is essential for a long service life. Herein, a material design is proposed to combine all these desirable attributes in a single artificial muscle platform. The design involves the molecular engineering of a liquid crystalline network with crystallizable segments and an ethylene glycol flexible spacer. A high degree of crystallinity can be afforded by utilizing aza-Michael chemistry to produce a low covalent crosslinking density, resulting in crack-insensitivity with a high fracture energy of 33 720 J m -2 and a high fatigue threshold of 2250 J m -2 . Such crack-resistant artificial muscle with tissue-matched modulus of 0.7 MPa can generate a high power density of 450 W kg -1 at a low temperature of 40 °C. Notably, because of the presence of crystalline domains in the actuated state, no crack propagation is observed after 500 heating-cooling actuation cycles under a static load of 220 kPa. This study points to a pathway for the creation of artificial muscles merging seemingly disparate, but desirable properties, broadening their application potential in smart devices., (© 2024 The Authors. Advanced Materials published by Wiley‐VCH GmbH.)

Polymeric gel-based artificial muscles exhibiting tissue-matched Young's modulus (10 Pa-1 MPa) promise to be core components in future soft machines with inherently safe human-machine interactions. However, the ability to simultaneously generate fast, large, high-power, and long-lasting actuation in the open-air environment, has yet been demonstrated in this class of ultra-soft materials. Herein, to overcome this hurdle, the design and synthesis of a twisted and coiled liquid crystalline glycerol-organogel (TCLCG) is reported. Such material with a low Young's modulus of 133 kPa can surpass the actuation performance of skeletal muscles in a variety of aspects, including actuation strain (66%), actuation rate (275% s -1 ), power density (438 kW m -3 ), and work capacity (105 kJ m -3 ). Notably, its power density is 14 times higher than the record of state-of-the-art polymeric gels. No actuation performance degradation is detected in the TCLCG even after air exposure for 7 days, owing to the excellent water retention ability enabled by glycerol as co-solvent with water. Using TCLCG, mobile soft robots with extraordinary maneuverability in unstructured environments are successfully demonstrated, including a crawler showing fast bidirectional locomotion (0.50 mm s -1 ) in a small-confined space, and a roller that can escape after deep burying in sand., (© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.)