Hydrogels have emerged as promising materials for the construction of skin-like mechanical sensors. The common design of hydrogel-based artificial skin requires a dielectric sandwiched between two hydrogel layers for capacitive sensing. However, such a planar configuration limits the sensitivity, stretchability and self-healing properties. Here, we report the design of single-layer composite hydrogels with bulk capacitive junctions as mechanical sensors. We engineer dielectric peptide-coated graphene (PCG) to serve as homogenously dispersed electric double layers in hydrogels. Any mechanical motions that alter the microscopic distributions of PCG in the hydrogels can significantly change the overall capacitance. We use peptide self-assembly to render strong yet dynamic interfacial interactions between the hydrogel network and graphene. The resulting hydrogels can be stretched up to 77 times their original length and self-heal in a few minutes. The devices can effectively sense strain and pressure in both air and aqueous environments, providing tremendous opportunities for next-generation iontronics.

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Polycatenanes are extremely attractive topological architectures on account of their high degrees of conformational freedom and multiple motion patterns of the mechanically interlocked macrocycles. However, exploitation of these peculiar structural and dynamic characteristics to develop robust catenane materials is still a challenging goal. Herein, we synthesize an oligo[2]catenane that showcases mechanically robust properties at both the microscopic and macroscopic scales. The key feature of the structural design is controlling the force-bearing points on the metal-coordinated core of the [2]catenane moiety that is able to maximize the energy dissipation of the oligo[2]catenane via dissociation of metal-coordination bonds and then activation of sequential intramolecular motions of circumrotation, translation, and elongation under an external force. As such, at the microscopic level, the single-molecule force spectroscopy measurement exhibits that the force to rupture dynamic bonds in the oligo[2]catenane reaches a record high of 588 ± 233 pN. At the macroscopic level, our oligo[2]catenane manifests itself as the toughest catenane material ever reported (15.2 vs 2.43 MJ/m 3 ). These fundamental findings not only deepen the understanding of the structure-property relationship of poly[2]catenanes with a full set of dynamic features but also provide a guiding principle to fabricate high-performance mechanically interlocked catenane materials.