Stretchable electrodes are playing important roles in the measurement of bio‐electrical signals especially in wearable electronic devices. These electrodes usually adopt commercial elastomers such as polydimethylsiloxane or polystyrene‐ethylene‐butylene‐styrene as substrates, which result in poor stability and reliability due to weak interfacial adhesion between electrodes and human skin. Here, dopamine is introduced into the hydrogen bonding based elastomer as pendent groups. The elastomer shows both mechanical strength and adhesion strength at the same time. It exhibits high stress at break (1.9 MPa) and high fracture strain (5100%). Significantly, it exhibits a high adhesive strength (≈62 kPa) and underwater adhesive strength (≈16 kPa) with epithelial tissue. Thus, a stretchable bio‐interfacial electrode is fabricated by spray‐coating silver nanowires on the elastic substrate, which is stretchable, self‐healable, and highly adhesive and suitable for electromyogram measurement.

Conductive hydrogels (CHs) are regarded as one of the most promising materials for bioelectronic devices on human‐machine interfaces (HMIs). However, conventional CHs cannot conform well with complex skin surfaces, such as hairy or wrinkled skin, due to pre‐formation and insufficient adhesion; they also usually lack antibacterial abilities and require tissue‐harm and time‐consuming preparation (e.g., heating or ultraviolet irradiation), which limits their practical application on HMIs. Herein, an in situ forming CH is proposed by taking advantage of the PEDOT:PSS‐promoted self‐polymerization of zwitterionic [2‐(methacryloyloxy)ethyl]dimethyl‐(3‐sulfopropyl) (SBMA). The hydrogel is formed spontaneously after injection of the precursor solution onto the desired location without any additional treatments. The as‐prepared hydrogel possesses excellent elasticity (elastic recovery >96%), desirable adhesive strength (≈6.5 kPa), biocompatibility, and intrinsically antibacterial properties. Without apparent heat release (<5 °C) during gelation, the hydrogel can form in situ on skin. Additionally, the obtained hydrogel can establish tight contact with skin, forming highly conformal interfaces on hairy skin surfaces and irregular wounds. Finally, the in situ forming hydrogels are applied as conformal epidermal electrodes to record stable and reliable surface electromyogram signals from hairy skin (with high signal‐to‐noise ratio, SNR ≈ 32 dB) and accelerate diabetic wound healing under electrical stimulation.

Silicon is expected to become the ideal anode material for the next generation of high energy density lithium battery because of its high theoretical capacity (4200 mAh g −1 ). However, for silicon electrodes, the initial coulombic efficiency (ICE) is low and the volume of the electrode changes by over 300% after lithiation. The capacity of the silicon electrode decreases rapidly during cycling, hindering the practical application. In this work, a slidable and highly ionic conductive flexible polymer binder with a specific single-ion structure (abbreviated as SSIP) is presented in which polyrotaxane acts as a dynamic crosslinker. The ionic conducting network is expected to reduce the overall resistance, improve ICE and stabilize the electrode interface. Furthermore, the introduction of slidable polyrotaxane increases the reversible dynamics of the binder and improves the long-term cycling stability and rate performance. The silicon anode based on SSIP provides a discharge capacity of ≈1650 mAh g −1 after 400 cycles at 0.5C with a high ICE of upto 92.0%. Additionally, the electrode still exhibits a high ICE of 87.5% with an ultra-high Si loading of 3.84 mg cm −2 and maintains a satisfying areal capacity of 5.9 mAh cm −2 after 50 cycles, exhibiting the potential application of SSIP in silicon-based anodes.

A series of stretchable single-ion polymer electrolytes (SIPEs) based on Pluronic and 2-acrylamido-2-methylpropane sulfonic lithium (AMPS) are presented. Owing to the microphase separation of the soft segment and hard segment, this SIPE family exhibits high stretchability in which SIPE-2 can be stretched up to 840% with a fracture strength of 7.40 MPa. High Li+ content (2.06 wt %) is rationally incorporated via covalently grafting AMPS segments onto the polymer backbone, and therefore, these quasi-solid-state SIPEs delivers a considerable ionic conductivity of 1.10 × 10–4 S cm–1 at 65 °C, a wide electrochemical stability window (>5.0 V), and a high lithium transfer number (t Li+ > 0.93). Consequently, the stretchable and highly conductive single-ion polymer electrolytes show great potential for stretchable and flexible batteries.

Lightweight aerogels with elastic performance and tunable surface properties have made them a good alternative for smart electornic skin. However, the aerogels remain a great barrier for sensing applications because of their severe brittleness and difficult regulation of surface property. Herein, we report a superelastic aerogel originated from a rational designed waterborne poly­(siloxane-benzoxazine) by using the ice template method. The three-dimensional (3D) network is constructed via the radical crosslinking and ring-opening polymerization followed by the freeze-drying process. Moreover, it also shows pronounced mechanical performance that can be compressed over 70% and recover without fracture. Beyond that, its surface property could be altered from highly hydrophilic to hydrophobic property (145° water contact angle) by adjusting the crosslinking degree of the aerogel under different curing temperatures. We further demonstrate a pressure sensor by in situ polymerization of the aniline (PANI) on the surface of the aerogel. The multifunctional properties make it an attractive material for self-cleaning electronic skin.