Regulating the Stable Lithium and Polysulfide Deposition in Batteries by a Gold Nanoparticle Modified Vertical Graphene Host

3D hosts have been widely investigated to stabilize the lithium (Li) metal anode (LMA) for next‐generation high‐energy‐density batteries. However, the complicated porous structure and the lithiophobic framework always lead to nonuniform Li deposition and low host utilization. Herein, Au nanoparticle (NP)–modified vertical graphenes, which are grown on flexible graphite paper, are prepared as the 3D host (denoted Au‐VG‐GP) to guide Li nucleation and deposition. It is shown that the vertical graphene structure with the low tortuosity effectively decreases the ion diffusion resistance and avoids the formation of a concentration gradient, ensuring uniform ion distribution in the 3D host. At the same time, the uniformly distributed Au NPs act as heterogeneous seeds guiding fast and uniform Li nucleation and growth. As a result, the Au‐VG‐GP host effectively stabilizes the LMA and achieves a high Coulombic efficiency in the half‐cells. A small overpotential and long cycling stability are also achieved for the LMA in the symmetrical cells and full batteries with such a host. In addition, such a host can also guide uniform and high‐capacity deposition of Li 2 S in the cathode of lithium–sulfur batteries, showing its potential uses in energy storage devices based on a dissolution–deposition mechanism.