The world’s mounting demands for environmentally benign and efficient resource utilization have spurred investigations into intrinsically green and safe energy storage systems. As one of the most promising types of batteries, the Zn battery family, with a long research history in the human electrochemical power supply, has been revived and reevaluated in recent years. Although Zn anodes still lack mature and reliable solutions to support the satisfactory cyclability required for the current versatile applications, many new concepts with optimized Zn/Zn2+ redox processes have inspired new hopes for rechargeable Zn batteries. In this review, we present a critical overview of the latest advances that could have a pivotal role in addressing the bottlenecks (e.g., nonuniform deposition, parasitic side reactions) encountered with Zn anodes, especially at the electrolyte-electrode interface. The focus is on research activities towards electrolyte modulation, artificial interphase engineering, and electrode structure design. Moreover, challenges and perspectives of rechargeable Zn batteries for further development in electrochemical energy storage applications are discussed. The reviewed surface/interface issues also provide lessons for the research of other multivalent battery chemistries with low-efficiency plating and stripping of the metal.Zinc batteries: Improving performance using novel electrolytesUsing novel functional electrolytes to stabilize zinc batteries could help power technology including wearable electronics without the costs and hazards of lithium-ion devices. Jingwen Zhao and Guanglei Cui from the Chinese Academy of Sciences in Qingdao review how the performance of zinc batteries, which have high energy storage but unsatisfactory cyclability, can be improved through modified electrolytes that limit unwanted (electro)chemical processes. Especially, a shift from water-based electrolytes towards polymers can tremendously extend zinc battery lifetimes, while simultaneously enabling packaging into devices. Other approaches include coating electrodes with polymers or inorganic materials to encourage uniform zinc deposition during recharging. Electrodes that combine zinc with carbon fibers, or form the metal into 3D sponges, can also ensure reliable recharging.