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The unstable lithium (Li)/electrolyte interface, causing inferior cycling efficiency and unrestrained dendrite growth, has severely hampered the practical deployment of Li metal batteries (LMBs), particularly in carbonate electrolytes. Herein, we present a robust approach capitalizing on a dynamic supramolecular elastomer (DSE) interface layer, which is capable of being reduced with Li metal to spontaneously form strong Li+ion-dipole interaction, thereby enhancing interfacial stability in carbonate electrolytes. The soft phase in the DSE structure enables fast Li+transport via loosely coordinated Li+–O interaction, while the hard phase, rich in electronegative lithiophilic sites, drives the generation of fast-ion-conducting solid electrolyte interface components, including Li3N and Li2S. Furthermore, the dynamically resilient DSE network composed of soft and hard phases protects Li anodes from electrolyte corrosion and accommodates volume changes during cycling. All features of the DSE layer synergistically facilitate uniform Li+deposition and suppress Li dendrite propagation, ensuring a stable and dendrite-free Li anode. Consequently, the symmetric Li||Li cell incorporating the DSE layer achieves cycling stability exceeding 6000 h under 1 mA cm–2and 1 mA h cm–2conditions. Furthermore, full cell pairing DSE/Li anode with LiFePO4(LFP) or high-voltage LiNi0.8Mn0.1Co0.1O2(NMC811) cathodes exhibits high-efficiency Li deposition and cycling stability, even under constrained conditions of limited Li (40 μm) and ultrahigh loading NMC811 cathode (21.5 mg cm–2). This study underscores the effectiveness of the ion-dipole interaction-enabled DSE network in developing stable, high-energy-density LMBs.

Building 3D electron-conducting scaffolds has been proven to be an effective way to alleviate severe dendritic growth and infinite volume change of sodium (Na) metal anodes. However, the electroplated Na metal cannot completely fill these scaffolds, especially at high current densities. Herein, we revealed that the uniform Na plating on 3D scaffolds is strongly related with the surface Na+conductivity. As a proof of concept, we synthesized NiF2hollow nanobowls grown on nickel foam (NiF2@NF) to realize homogeneous Na plating on the 3D scaffold. The NiF2can be electrochemically converted to a NaF-enriched SEI layer, which significantly reduces the diffusion barrier for Na+ions. The NaF-enriched SEI layer generated along the Ni backbones creates 3D interconnected ion-conducting pathways and allows for the rapid Na+transfer throughout the entire 3D scaffold to enable densely filled and dendrite-free Na metal anodes. As a result, symmetric cells composed of identical Na/NiF2@NF electrodes show durable cycle life with an exceedingly stable voltage profile and small hysteresis, particularly at a high current density of 10 mA cm–2or a large areal capacity of 10 mAh cm–2. Moreover, the full cell assembled with a Na3V2(PO4)3cathode exhibits a superior capacity retention of 97.8% at a high current of 5C after 300 cycles.