The development of stretchable strain sensors is crucial for the implementation of electronic skins and wearable electronics. Resistive‐type strain sensors are typically composed of an electrically conductive sensing layer coupled to a stretchable substrate. When a sensor is stretched, microstructural changes in the sensing layer lead to a strain‐dependent change in resistance. However, strain sensors with high sensitivity and specificity often suffer from a limited detection range along with reliability issues. Here, a novel strain sensor composed of Ag particles and long‐range entangled carbon nanotubes (CNTs) with a special composite design is proposed, in which a strain‐induced self‐locking effect is introduced at the interface between the CNT film and a percolating network consisting of Ag particle filler. As a result, the sensors achieve significantly enhanced performance such as large stretchability (≥120%), high gauge factor (3990.8), fast response time (<33 ms), and high mechanical durability. A range of wearable applications including radial artery, facial expression, and joint motion monitoring are demonstrated, which range from minute deformation to excessive stretching of the sensor.

Transparent, conductive hydrogels with good mechanical strength and toughness are in great demand of the fields of biomedical and future wearable smart electronics. We reported a carboxymethyl chitosan (CMCS)–calcium chloride (CaCl2)/polyacrylamide (PAAm)/poly(N-methylol acrylamide (PNMA) transparent, tough and conductive hydrogel containing a bi-physical crosslinking network through in situ free radical polymerization. It showed excellent light transmittance (>90%), excellent toughness (10.72 MJ/m3), good tensile strength (at break, 2.65 MPa), breaking strain (707%), and high elastic modulus (0.30 MPa). The strain sensing performance is found with high sensitivity (maximum gauge factor 9.18, 0.5% detection limit), wide strain response range, fast response and recovery time, nearly zero hysteresis and good repeatability. This study extends the transparent, tough, conductive hydrogels to provide body-surface wearable devices that can accurately and repeatedly monitor the movement of body joints, including the movements of wrists, elbows and knee joints. This study provided a broad development potential for tough, transparent and conductive hydrogels as body-surface intelligent health monitoring systems and implantable soft electronics.

Robust conductive hydrogels are in great demand for the practical applications of smart soft robots, epidermal electronics, and human–machine interactions. We successfully prepared nanoparticles enhanced polyacrylamide/hydroxypropyl guar gum/acryloyl-grafted chitosan quaternary ammonium salt/calcium ions/SiO2 nanoparticles (PHC/Ca2+/SiO2 NPs) conductive hydrogels. Owing to the stable chemical and physical hybrid crosslinking networks and reversible non-covalent interactions, the PHC/Ca2+/SiO2 NPs conductive hydrogel showed good conductivity (~3.39 S/m), excellent toughness (6.71 MJ/m3), high stretchability (2256%), fast self-recovery (80% within 10 s, and 100% within 30 s), and good fatigue resistance. The maximum gauge factor as high as 66.99 was obtained, with a wide detectable strain range (from 0.25% to 500% strain), the fast response (25.00 ms) and recovery time (86.12 ms), excellent negligible response hysteresis, and good response stability. The applications of monitoring the human’s body movements were demonstrated, such as wrist bending and pulse tracking.

Conductive hydrogels are widely used in sports monitoring, healthcare, energy storage, and other fields, due to their excellent physical and chemical properties. However, synthesizing a hydrogel with synergistically good mechanical and electrical properties is still challenging. Current fabrication strategies are mainly focused on the polymerization of hydrogels with a single component, with less emphasis on combining and matching different conductive hydrogels. Inspired by the gradient modulus structures of the human skin, we propose a bilayer structure of conductive hydrogels, composed of a spray-coated poly(3,4-dihydrothieno-1,4-dioxin): poly(styrene sulfonate) (PEDOT:PSS) as the bonding interface, a relatively low modulus hydrogel on the top, and a relatively high modulus hydrogel on the bottom. The spray-coated PEDOT:PSS constructs an interlocking interface between the top and bottom hydrogels. Compared to the single layer counterparts, both the mechanical and electrical properties were significantly improved. The as-prepared hydrogel showed outstanding stretchability (1763.85 ± 161.66%), quite high toughness (9.27 ± 0.49 MJ/m3), good tensile strength (0.92 ± 0.08 MPa), and decent elastic modulus (69.16 ± 8.02 kPa). A stretchable strain sensor based on the proposed hydrogel shows good conductivity (1.76 S/m), high sensitivity (a maximum gauge factor of 18.14), and a wide response range (0–1869%). Benefitting from the modulus matching between the two layers of the hydrogels, the interfacial interlocking network, and the patch effect of the PEDOT:PSS, the strain sensor exhibits excellent interface robustness with stable performance (>12,500 cycles). These results indicate that the proposed bilayer conductive hydrogel is a promising material for stretchable electronics, soft robots, and next-generation wearables.

Conformable, sensitive, long-lasting, external power supplies-free multifunctional electronics are highly desired for personal healthcare monitoring and artificial intelligence. Herein, we report a series of stretchable, skin-like, self-powered tactile and motion sensors based on single-electrode mode triboelectric nanogenerators. The triboelectric sensors were composed of ultraelastic polyacrylamide (PAAm)/(polyvinyl pyrrolidone) PVP/(calcium chloride) CaCl2 conductive hydrogels and surface-modified silicon rubber thin films. The significant enhancement of electrospun polyvinylidene fluoride (PVDF) nanofiber-modified hierarchically wrinkled micropyramidal architectures for the friction layer was studied. The mechanism of the enhanced output performance of the electrospun PVDF nanofibers and the single-side/double-side wrinkled micropyramidal architectures-based sensors has been discussed in detail. The as-prepared devices exhibited excellent sensitivity of a maximum of 20.1 V/N (or 8.03 V/kPa) as tactile sensors to recognize a wide range of forces from 0.1 N to 30 N at low frequencies. In addition, multiple human motion monitoring was demonstrated, such as knee, finger, wrist, and neck movement and voice recognition. This work shows great potential for skin-like epidermal electronics in long-term medical monitoring and intelligent robot applications.