Jiaxin Ma, Zhong-Shuai Wu*

Science Bulletin, 2026, accepted.

In this Research Highlight, we focus on the conceptual significance of cross-electrode coupling chemistry in stabilizing anode-free lithium metal batteries. We highlight the intrinsic limitations of conventional interfacial regulation strategies, particularly their reliance on localized regulation that overlooks the coupled nature of electrochemical processes. The discussion outlines a shift toward system-level interfacial design and emphasizes the role of electrolyte-mediated interactions in governing interphase formation. By connecting interphase characteristics with lithium deposition behavior, this work identifies planar lithium dynamics as a key feature of interfacial stability and further relates these features to the demonstrated device-level performance, including anode-free pouch cells with extended cycle life under practical conditions.