In Situ Grown Silver–Polymer Framework with Coordination Complexes for Functional Artificial Tissues

Abstract Self‐sensing actuators are critical to artificial robots with biomimetic proprio‐/exteroception properties of biological neuromuscular systems. Existing add‐on approaches, which physically blend heterogeneous sensor/actuator components, fall short of yielding satisfactory solutions, considering their suboptimal interfaces, poor adhesion, and electronic/mechanical property mismatches. Here, a single homogeneous material platform is reported by creating a silver–polymer framework (SPF), thus realizing the seamless sensing–actuation unification. The SPF‐enabled elastomer is highly stretchable (1200%), conductive (0.076 S m⁻¹), and strong (0.76 MPa in‐strength), where the stretchable polymer matrix synthesis and in situ silver nanoparticles reduction are accomplished simultaneously. Benefiting from the multimodal sensing capability from its architecture itself (mechanical and thermal cues), self‐sensing actuation (proprio‐deformations and external stimuli perceptions) is achieved for the SPF‐based pneumatic actuator, alongside an excellent load‐lifting attribute (up to 3700 times its own weight), substantiating its advantage of the unified sensing–actuation feature in a single homogenous material. In view of its human somatosensitive muscular systems imitative functionality, the reported SPF bodes well for use with next‐generation functional tissues, including artificial skins, human–machine interfaces, self‐sensing robots, and otherwise dynamic materials.