The formation of lithium dendrites induces the notorious safety issue and poor cycling life of energy storage devices, such as lithium–sulfur and lithium–air batteries. We propose a surface energy model to describe the complex interface between the lithium anode and electrolyte. A universal strategy of hindering formation of lithium dendrites via tuning surface energy of the relevant thin film growth is suggested. The merit of the novel motif lies not only fundamentally a perfect correlation between electrochemistry and thin film fields, but also significantly promotes larger‐scale application of lithium–sulfur and lithium–air batteries, as well as other metal batteries (e.g., Zn, Na, K, Cu, Ag, and Sn).

Metal–organic frameworks (MOFs) are promising materials for batteries and supercapacitors. However, random crystal orientations and low conductivity can result in poor performance. Designing a convenient method to address these issues is therefore an important challenge. Here we describe an efficient strategy to fabricate self-supported MOF wall-like architectures with uniform orientation on carbon nanowalls (CNWs) as seedbeds. In addition, we gain molecular-level insight into the interface between CNWs and MOF nanosheets using density functional theory calculations. Our results suggest that assembled ions anchor on edge carbon atoms to match the matrix of the edges of CNWs, while the remaining ions self-assemble with terminal –COOH groups on p-benzenedicarboxylic acid ligands to form the structure. Our findings demonstrate a feasible method to fabricate integrated MOF electrodes with ideal orientations and, therefore, may pave the way to unlock the inherent high performance of MOF materials towards a number of engineering applications.