Intelligent skinlike materials have recently attracted tremendous research interests for employing in electronic skin, soft robotics, and wearable devices. Because the traditional soft matters are restricted in unsatisfactory mechanical performances or short-term usage, these materials are adverse to practical applications. Here, intriguing conductive hydrogel materials with multifunctionality (MFHs) are fabricated by using poly­(acrylic acid) (PAA), dopamine-functionalized hyaluronic acid (DHA), and Fe3+ as ionic cross-linker. The mussel-inspired networks with delicate combination of physical and chemical cross-linking possess synergistic features of inherent viscoelasticity, high stretchability (800%), and durable self-adhesiveness to various substrates. Owing to the abundant hydrogen bonds and multiple metal coordination interactions between Fe3+, catechol, and carboxylic groups, the matrix reveals repeatable thermoplasticity and autonomous self-healing property both mechanically and electrically (98% recovery in 2 s). When served as strain sensors, the MFHs can distinctly perceive complex body motions from tiny physiological signal (breathing) to large movements (knee bending) as human motion detecting devices. Moreover, the MFHs were explored as ideal material for circuit repairing, programming, and switches constructing because of their excellent properties. Consequently, these eco-friendly hydrogel ionotronic devices can be promising candidates for next-generation intelligent wearable devices and human–machine interfaces.

Amphiphilic derivatives of fullerene C60 are attractive from viewpoints of supramolecular chemistry and biomedicine. The establishment of relationships among the molecular structure, aggregation behavior and properties such as scavenging radicals of the amphiphilic C60 derivatives is the key to push these carbon nanomaterials to real applications. In this work, six monosubstituted C60 derivatives were synthesized by a one-step quaternization of their neutral precursors, which bear Percec monodendrons terminated with oligo­(poly­(ethylene oxide)) (o-PEO) chain(s). The main difference among the C60 derivatives lies in the number and substituted position of the o-PEO chain(s) within the Percec monodendron. Derivative with a 4-substitution of the o-PEO chain still showed limited solubility in water. Other derivatives possessing two or three o-PEO chains exhibited much improved solubilities and rich aggregation behavior in water. It was found that the formation of aggregates is regulated both by the number and the substituted pattern of the o-PEO chains. Typical morphologies include nanosheets, nanowires, vesicles, nanotubes, and nanorods. Although the structures of the C60 derivatives are different from those of traditional surfactants, their aggregation behavior can be also well explained by applying the theory of critical packing parameter. Interestingly, the capabilities of the C60 derivatives to scavenge the hydroxyl radicals (OH· –) followed the same order of their solubility in water, where the compound bearing three o-PEO chains with a 2,3,4-substitution got the champion quenching efficiency of ∼97.79% at a concentration of 0.15 mg·mL–1 (∼0.11 mmol·L–1).

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