Although current high-energy-density lithium-ion batteries (LIBs) have taken over the commercial rechargeable battery market, increasing concerns about limited lithium resources, high cost, and insecurity of organic electrolyte scale-up limit their further development. Rechargeable aqueous zinc-ion batteries (ZIBs), an alternative battery chemistry, have paved the way not only for realizing environmentally benign and safe energy storage devices but also for reducing the manufacturing costs of nextgeneration batteries. This Review underscores recent advances in aqueous ZIBs; these include the design of a highly reversible Zn anode, optimization of the electrolyte, and a wide range of cathode materials and their energy storage mechanisms. We also present recent advanced techniques that aim at overcoming the current issues in aqueous ZIB systems. This Review on the future perspectives and research directions will provide a guide for future aqueous ZIB study.

We retrospect recent advances in rechargeable aqueous zinc-ion batteries system and the facing challenges of aqueous zinc-ion batteries. Importantly, some concerns and feasible solutions for achieving practical aqueous zinc-ion batteries are discussed in detail.

We report a new class of Zn anodes modified by a three-dimensional nanoporous ZnO architecture (Zn@ZnO-3D), which can accelerate the kinetics of Zn2+ transfer and deposition, inhibit dendrite growth, and reduce the side-reactions.

Aqueous zinc‐ion batteries are largely restricted by the unsatisfactory performance of zinc (Zn) anodes, including their poor stability and irreversibility. In particular, the mechanism behind the electrochemical contrast caused by the surface crystal plane, which is a decisive factor of the electrochemical characteristics of the hostless Zn anode, is still relatively indistinct. Hence, new insight into a novel anode with a surface‐preferred (002) crystal plane is provided. The interfacial reaction and morphology evolution are revealed by theoretical analysis and post‐mortem/operando experimental techniques, indicating that Zn anodes with more exposed (002) basal planes exhibit free dendrites, no by‐products, and weak hydrogen evolution, in sharp contrast to the (100) plane. These features benefit the Zn (002) anode by enabling a long cyclic life of more than 500 h and a high average coulombic efficiency of 97.71% for symmetric batteries, along with delivering long cycling stability and reversibility with life spans of over 2000 cycles for full batteries. This work provides new insights into the design of high‐performance Zn anodes for large‐scale energy storage and can potentially be applied to other metal anodes suffering from instability and irreversibility.

Rechargeable aqueous zinc‐ion batteries (ZIBs) featuring the merits of low cost, eco‐friendliness, and enhanced safety have attracted extensive interests and considered as the most promising energy storage system. However, much efforts are devoted to the exploration of cathode materials and their storage mechanisms in this system, and inadequate attentions are received in regard to anode side especially in neutral or mild acidic electrolyte. Therefore, in this review, the fundamental understanding of existing issues including dendrite formation, corrosion, and hydrogen evolution are mainly revealed, as well as their interaction in neutral or mild acidic medium. In addition, the currently existing solution strategies on the anode are summarized and the mechanisms that contained are simultaneously investigated. Finally, perspectives on future anode modification and innovation direction are provided for the further development and research of Zn‐based ZIBs.