Lithium batteries (LBs) are developed tremendously owing to their excellent energy density as well as cyclic persistence, exhibiting promising applications from portable devices to e‐transportation and grid fields. However, with the ever‐increasing demand for intelligent wearable electronics, more requests are focused on high safety, good durability, and satisfied reliability of LBs. The self‐healing route, which can simulate the ability of organic organisms to repair damage and recover initial function through its intrinsic vitality, is believed to be an efficient strategy to alleviate the unavoidable physical or chemical fatigue and damage issues of LBs, beneficial for the realization of the above mentioned high requests. In this review, the applicability and development of self‐healing materials are summarized in electrodes, electrolytes, and interfacial layers in recent years, focusing on exploring the feasibility of different self‐healing strategies in LBs, discussing the advantages and disadvantages of existing strategies in different parts of batteries, and indicating the possible research directions for beginners who are interested in this field. Finally, the critical challenges and the future research directions as well as opportunities are prospected.

Lithium-ion batteries (LIBs) with high energy density and fastcharge capability are urgently required for the ever-growing demands for electric vehicles and hybrid electric vehicles. To achieve this demand, as one of the important components, electrolytes are required to work well at a high voltage to fulfill the good performance of high energy density batteries and facilitate the fast-charge process. In this review, we mainly focus on the electrolytes design for LIBs under high-voltage and fast-charge conditions. The bottlenecks and the typical resolving strategies referring to lithium salts, solvents, solid electrolyte interface, additives and solvent structures in electrolytes are presented in detail. Finally, we propose the challenges regarding electrolytes design insight and inspiration for LIBs under the two conditions to give a better guide for the rationale design of the high energy density and fast-charge devices in the future applications.