摘要：This vertically self‐pillared(VSP)structure extends the application range of traditional porous materials with facile mass/ion transport and enhanced reaction ***,we prepare a single crystal metal‐organic framework(MOF),employing the ZIF‐67 structure as a proof of concept,which is constructed by vertically self‐pillared nanosheets(VSP‐MOF).We further converted VSP‐MOF into VSP‐cobalt sulfide(VSP‐CoS2)through a sulfidation *** plays an important role in almost all battery technologies;for metallic batteries,lithium anodes exhibit a high theoretical specific capacity,low density,and low redox ***,during the half‐cell reaction(Li++e=Li),uncontrolled dendritic Li penetrates the separator and solid electrolyte interphase *** employed as a composite scaffold for lithium metal deposition,there are many advantage to using this framework:1)the VSP‐CoS2 substrate provides a high specific surface area to dissipate the ion flux and mass transfer and acts as a pre‐catalyst,2)the catalytic Co center favors the charge transfer process and preferentially binds the Li+with the enhanced electrical fields,and 3)the VSP structure guides the metallic propagation along the nanosheet 2D orientation without the protrusive *** these features enable the VSP structure in metallic batteries with encouraging performances.