High power density and fast charging batteries are instrumental in the transition to electrified aerial, maritime, and terrestrial transportation. Charge-transfer across interfaces of battery components plays a critical role in dictating charging/discharging kinetics where suboptimal Li-ion ) transfer is a significant bottleneck impeding the performance of the battery. This interface challenge pertains to both traditional and emerging Li-ion battery chemistries, including liquid -as well as solid -state electrolytes. Although interfacial engineering-via, e.g., advanced electrolyte formulations, surface modifications, and surface coatings -has attracted substantial interest in the battery community in recent years, it remains a relatively underexplored area in the pursuit of rational battery design. Thus, enhancing the atomic-to macrolevel understanding of the interplay between electrode materials and electrolytes can provide guidance towards improved performance and lifespan of batteries.