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Although the highest theoretical specific capacity and lowest redox potential make lithium metal anodes essential for next‐generation high‐energy batteries, the infinite volume changes and uncontrollable Li dendrites severely restrict their application. Herein, the 3D hierarchical framework (3DHF) loaded with lithiophilic nanorod arrays on interwoven carbon fibers is constructed as a host to stabilize the Li metal anode. With cooperation of the lithiophilicity and the capillary force of the nanorod arrays, molten Li easily wraps the surface of the nanorods to form 3DHF−Li composite anodes. The void spaces and channels among the nanorods may provide a buffer space for Li stripping/plating to relieve the volume changes. In addition, the enlarged specific surface area reduces the local current density to homogenize Li deposition and suppress Li dendrites. The 3DHF−Li anodes exhibit improved cycle stability and rate capability in both symmetric cells and full cells, providing references for the development of Li composite anodes.

The Cover Feature illustrates the Li stripping/plating behaviors on the 3D lithiophilic nanorod arrays structure. The nanorod arrays supply a large number of Li deposition sites. The abundant channels along nanorods provide sufficient buffer space for Li deposition and Li+ dissolution, and thus suppress the volume change and promote non‐dendritic Li plating. As a result, the Li composite electrode with the 3D hierarchical host exhibits excellent electrochemical properties. More information can be found in the Article by W. Chen et al.