The current boom of safe and renewable energy storage systems is driving the recent renaissance of Zn‐ion batteries. However, the notorious tip‐induced dendrite growth on the Zn anode restricts their further application. Herein, the first demonstration of constructing a flexible 3D carbon nanotube (CNT) framework as a Zn plating/stripping scaffold is constituted to achieve a dendrite‐free robust Zn anode. Compared with the pristine deposited Zn electrode, the as‐fabricated Zn/CNT anode affords lower Zn nucleation overpotential and more homogeneously distributed electric field, thus being more favorable for highly reversible Zn plating/stripping with satisfactory Coulombic efficiency rather than the formation of Zn dendrites or other byproducts. As a consequence, a highly flexible symmetric cell based on the Zn/CNT anode presents appreciably low voltage hysteresis (27 mV) and superior cycling stability (200 h) with dendrite‐free morphology at 2 mA cm−2, accompanied by a high depth of discharge (DOD) of 28%. Such distinct performance overmatches most of recently reported Zn‐based anodes. Additionally, this efficient rechargeability of the Zn/CNT anode also enables a substantially stable Zn//MnO2 battery with 88.7% capacity retention after 1000 cycles and remarkable mechanical flexibility.

Rechargeable aqueous zinc‐based batteries (AZBs) have been recently considered as desirable energy storage devices for renewable energy storage because of their high theoretical capacity, low cost, and high safety. Despite the inspiring achievements in this field, the energy density of AZBs is still far below expectation, which directly hinders their practical application as next‐generation secondary cells. To address this issue, previously, reseach efforts have been mainly dedicated to the improvement of capacity by designing different kinds of high‐capacity electrode candidates, especially the cathode materials. In recent years, elevation of the output voltage for energy density improvement has gained more and more attention. The main limitation of the relatively low output voltage of AZBs lies in the narrow electrochemically stable window of aqueous electrolytes, which results in limited choice of cathode materials with high potential. Herein, by summarizing recently reported work in this field, the strategies applied to high‐voltage AZB construction are classified into two categories, from the aspects of electrode and battery structure. Classic examples of each category are discussed in detail, and their respective advantages/defects are compared and commented on. Finally, further challenges are elaborated to provide more insights into this area.

The relatively low energy density and poor cycling durability of aqueous rechargeable Co–Zn batteries are two main bottlenecks impeding their application in next-generation energy storage devices. A traditional solution for this issue is preparing complicated three-dimensional (3D) electrodes on conductive substrates by epitaxial growth, whose active material easily falls off. Herein, an aqueous rechargeable Co–Zn battery with ultrahigh energy density and excellent electrochemical reversibility is constructed by employing an ultrasonic-assisted growth of a Co­(OH)2 nanosheet on Co foam (denoted as COHF) as the cathode. Taking advantage of in-situ formed electrochemically active Co­(OH)2 and a porous 3D conductive framework, the COHF electrode presents an ultrahigh capacity of 0.265 mA h cm–2, 24-fold higher than that of pristine Co foam. Impressively, a remarkable energy density of 6.09 mW h cm–3 and a peak power density of 1.75 W cm–3 are achieved by the as-fabricated COHF//Zn battery. Moreover, this COHF//Zn battery exhibits an admirable cyclic durability with 83.3% capacity retention after 10 000 cycles.

Antimony (Sb) holds a high theoretic capacity and suitable redox potential as a promising anode for aqueous alkaline batteries (AABs). However, the uncontrollable nucleation for SbO2− and promiscuous water‐induced side reactions severely degrade the reversibility of Sb anode. Herein, the carbon‐anchored Sb nanoparticles are constructed to induce uniform Sb plating/stripping for high‐performance AABs. The experimental results reveal that the enhanced interaction between carbon and antimony as well as defective carbon can significantly improve the electrical conductivity and decrease the Sb nucleation overpotential. Accordingly, the as‐prepared Sb anode enables preferential plating of Sb rather than parasitic side reactions. As a result, the cycle life of A‐Sb/CF is sustained over 500 cycles at 10 mA cm−2/2 mAh cm−2. Even at the high capacity of 4 mAh cm−2, this anode can cycle stably for 225 cycles, which is significantly better than the Sb/CF counterpart. Furthermore, the assembled Ni3S2@Ni(OH)2//A‐Sb/CF full battery demonstrates a high capacity of 2.17 mAh cm−2 and a stable cycle life of over 500 cycles.