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Dendrites and dead lithium formation over prolonged cycling have long been challenges that hinder the safe implementation of metallic Li anodes. Herein, we employ polymer-stabilized liquid metal nanoparticles (LM-P NPs) of eutectic gallium indium (EGaIn) to create uniform Li nucleation sites enabling homogeneous lithium electrodeposition. Block copolymers of poly­(ethylene oxide) and poly­(acrylic acid) (PEO-b-PAA) were grafted onto the EGaIn surface, forming stabilized, well-dispersed NPs. Using a scalable spray coating approach, LM-P NPs were fabricated on copper current collectors, providing lithiophilic PEO sites and interactive carboxyl groups to guide Li deposition. The Li-EGaIn alloying process greatly reduced the Li+ diffusion barrier, enabling fast Li transport through the coating layer, resulting in decreased nucleation overpotential. Therefore, about five times lower Li nucleation overpotential was obtained on the LM-P modified Cu with an optimal composition of the polymers than the bare Cu substrates. DFT computations was used to reveal the binding properties between the LM-P layer and Li. Due to the regulated Li plating/stripping process, as-obtained 30 μm Li anodes paired with LiNi0.8Co0.1Mn0.1O2 (NCM811) with a negative/positive electrode capacity (N/P) ratio ∼ 10 exhibited stable cycling performance at 0.5C for over 250 cycles, with an average Coulombic efficiency of 99.55%. Ultrathin Li (1 μm) anodes with an N/P ratio ∼ 0.6 were also demonstrated in Li|LiFePO4 cells, which examined the stabilization of Li by LM-P NPs and monitored practical loadings of Li anodes that are close to anode-free systems.

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