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Advanced sensation and actuation abilities of various living organisms in nature have inspired researchers to design bioinspired self‐sensing soft actuators. However, the majority of conventional soft actuators primarily possess actuation capabilities while lacking a real‐time sensing signal feedback. Here, a promising strategy is reported to develop highly stretchable and conductive hydrogels for bioinspired self‐sensing soft actuators, which integrate actuation and strain‐sensing functions into a single materials system. The conductive hydrogels are designed and fabricated by in situ copolymerization of amino‐functionalized MXene‐encapsulated liquid metal nanodroplets (LM@A‐MXene) and poly(N‐isopropylacrylamide) hydrogels with controllable activated nanogels as nano‐cross‐linkers. The resulting hydrogel presents a compacted conducting network and highly porous microstructure, giving rise to robust integration of high conductivity, excellent strain sensitivity, broad stretchability, high stability, and fast response speed. Interestingly, the gradient network structure, formed by self‐precipitation of LM@A‐MXene, endows the hydrogel with shape‐programmable actuation, light‐driven remote control, and self‐sensing function. As a proof‐of‐concept application, the soft gripper based on the self‐sensing hydrogel actuators is developed, which can not only grasp, lift, and release objects, but also perceive every movement state by monitoring resistance changes. The proposed self‐sensing soft actuator can offer new insights for developing smart soft robotics and other artificial intelligent devices. [ABSTRACT FROM AUTHOR]

Sophisticated sensing and actuation capabilities of many living organisms in nature have inspired scientists to develop biomimetic somatosensory soft robots. Herein, the design and fabrication of homogeneous and highly conductive hydrogels for bioinspired somatosensory soft actuators are reported. The conductive hydrogels are synthesized by in situ copolymerization of conductive surface‐functionalized MXene/Poly(3,4‐ethylenedioxythiophene)/poly(styrenesulfonate) ink with thermoresponsive poly(N‐isopropylacrylamide) hydrogels. The resulting hydrogels are found to exhibit high conductivity (11.76 S m−1), strain sensitivity (GF of 9.93), broad working strain range (≈560% strain), and high stability after over 300 loading–unloading cycles at 100% strain. Importantly, shape‐programmable somatosensory hydrogel actuators with rapid response, light‐driven remote control, and self‐sensing capability are developed by chemically integrating the conductive hydrogels with a structurally colored polymer. As the proof‐of‐concept illustration, structurally colored hydrogel actuators are applied for devising light‐driven programmable shape‐morphing of an artificial octopus, an artificial fish, and a soft gripper that can simultaneously monitor their own motions via real‐time resistance variation. This work is expected to offer new insights into the design of advanced somatosensory materials with self‐sensing and actuation capabilities, and pave an avenue for the development of soft‐matter‐based self‐regulatory intelligence via built‐in feedback control that is of paramount significance for intelligent soft robotics and automated machines. [ABSTRACT FROM AUTHOR]