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Polymeric membranes are considered as promising materials to realize safe and long‐life lithium metal batteries (LMBs). However, they are usually based on soft 1D linear polymers and thus cannot effectively inhibit piercing of lithium dendrites at high current density. Herein, single lithium‐ion conducting molecular brushes (GO‐g‐PSSLi) are successfully designed and fabricated with a new 2D “soft–hard–soft” hierarchical structure by grafting hairy lithium polystyrenesulfonate (PSSLi) chains on both sides of graphene oxide (GO) sheets. The ultrathin GO‐g‐PSSLi membrane is further constructed by evaporation‐induced layer‐by‐layer self‐assembly of GO‐g‐PSSLi molecular brushes. Unlike conventional soft 1D linear polymeric structure, the rigid 2D extended aromatic structure of intralayer GO backbones can bear the shield effect of preventing the dendrites possibly generated at high current density from …