Zn powder anode possesses great versatility compared to the Zn foil counterpart, but the rough surface with a high surface area aggravates the corrosion and dendrite growth. Herein, a dendrite‐free and anti‐corrosive semi‐liquid Zn anode (SLA) is successfully fabricated based on Zn powder and a thickening agent. Benefiting from the rheological property, the unique anode effectively releases the stress induced by Zn plating, especially under high‐current densities. Meanwhile, the dual‐conductive medium, i.e., ionic and electronic, homogenizes the ion flux and allows the stripping/plating to occur within the entire anode. In a symmetric cell, the SLA anode exhibits stable electrochemical behavior with a prolonged lifespan at the current density of 5 mA cm−2/10 mA cm−2 under the capacity of 5 mAh cm−2/10 mAh cm−2. Improved durability of more than 5000 cycles is endowed when assembling an SLA anode with a vanadium‐based cathode. This study provides an electrode rheology‐based approach to overcome the stability challenge of powder anode for scale‐up manufacturing.

Hydrogel electrolytes are widely explored in Zn metal batteries for application in wearable electronics. While extensive studies have been conducted on optimizing the chemical structure and boosting the tensile elasticity, the mechanical stability of the hydrogel under repeated deformation is largely overlooked, leading to unsatisfactory performance at large cycling capacity. This work systematically analyzes the compressive fatigue‐resistance properties of the hydrogel electrolyte, revealing the critical roles of the salt and copolymer matrix on crack initiation and propagation. It shows that, on the premise of homogeneous Zn deposition, an improved anti‐fatigue property is essential to achieve high‐capacity Zn metal anodes. The optimal Zn(ClO4)2‐polyacrylamide/chitosan hydrogel electrolyte (C‐PAMCS) exhibits an unprecedented lifespan of 1500 h for Zn//Zn cells at a current density of 10 mA cm−2 and a high areal capacity of 10 mAh cm−2. The potential application of C‐PAMCS is exemplified in all‐flexible Zn‐ion batteries enabled by a flexible current collector consisting of a Ag nanowires embedded elastomer. This study provides the rationale under hydrogel electrolyte engineering toward advanced Zn‐ion battereis and the application in flexible devices.

Zn‐ion batteries (ZIBs) have gathered unprecedented interest recently benefiting from their intrinsic safety, affordability, and environmental benignity. Nevertheless, their practical implementation is hampered by low rate performance, inferior Zn2+ diffusion kinetics, and undesired parasitic reactions. Innovative solutions are put forth to address these issues by optimizing the electrodes, separators, electrolytes, and interfaces. Remarkably, polymers with inherent properties of low‐density, high processability, structural flexibility, and superior stability show great promising in tackling the challenges. Herein, the recent progress in the synthesis and customization of functional polymers in aqueous ZIBs is outlined. The recent implementations of polymers into each component are summarized, with a focus on the inherent mechanisms underlying their unique functions. The challenges of incorporating polymers into practical ZIBs are also discussed and possible solutions to circumvent them are proposed. It is hoped that such a deep analysis could accelerate the design of polymer‐derived approaches to boost the performance of ZIBs and other aqueous battery systems as they share similarities in many aspects.

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