A zwitterionic osmolyte hydrogel electrolyte (SPS–Zn) modulates Zn deposition and suppresses dendrite growth. Batteries with SPS–Zn show a long cycling life and the material can be used to prepare integrated i-skin for detecting physiological signals.

Aqueous zinc-ion hybrid supercapacitors (ZHSCs) represent one of the current research subjects because of their flame retardancy, ease of manufacturing, and exceptional roundtrip efficiency. With the evolution into real useful energy storage cells, the bottleneck factors of the corrosion and dendrite growth problems must be properly resolved for largely boosting their cycling life and energy efficiency. Herein, a natural polysaccharide strengthened hydrogel electrolyte (denoted as PAAm/agar/Zn­(CF3SO3)2) was engineered by designing an asymmetric dual network of covalently cross-linked polyacrylamide (denoted as PAAm) and physically cross-linked loose polysaccharide (e.g., agar) followed by intense uptake of Zn­(CF3SO3)2 aqueous electrolyte. In this polymeric matrix, the PAAm chains are responsible for constructing the soft domains to immobilize the water molecules, and the agar component boosts the mechanical performance (by using its inherent reversible sacrificial bonds) and favors the electrolyte ion transport. Due to these reasons, the as-designed hydrogel electrolyte effectively inhibits the zinc dendrite growth, realizes the uniform Zn deposition, and affords a satisfactory ionic conductivity of 1.55 S m–1, excellent tensile strength (78.9 kPa at 507.7% stretchable), and high compression strength (118.0 kPa at 60.0% strain). Additionally, a biopolymer-derived N-doped carbon microsphere cathode material with a highly interconnected porous carbonaceous network (denoted as NC) was also synthesized, which delivers a high capacity of 92.8 mAh g–1, along with superb rate capability and long duration cycling lifespan (95.4% retention for 10000 cycles) in the aqueous Zn//NC ZHSC. More notably, with integrated merits of the PAAm/agar/Zn­(CF3SO3)2 hydrogel electrolyte and NC, the as-built quasi-solid-state ZHSC achieves a high specific capacity of 73.4 mAh g–1 and superior energy density of 61.3 Wh kg–1 together with excellent cycling stability for 10000 cycles. This work demonstrated favorable practicability in the structural design of the hydrogel electrolytes and electrode materials for advanced ZHSC applications.