Facile Lithium Densification Kinetics by Hyperporous/Hybrid Conductor for High‐Energy‐Density Lithium Metal Batteries

Lithium metal anode (LMA) emerges as a promising candidate for lithium (Li)‐based battery chemistries with high‐energy‐density. However, inhomogeneous charge distribution from the unbalanced ion/electron transport causes dendritic Li deposition, leading to “dead Li” and parasitic reactions, particularly at high Li utilization ratios (low negative/positive ratios in full cells). Herein, an innovative LMA structural model deploying a hyperporous/hybrid conductive architecture is proposed on single‐walled carbon nanotube film (HCA/C), fabricated through a nonsolvent induced phase separation process. This design integrates ionic polymers with conductive carbon, offering a substantial improvement over traditional metal current collectors by reducing the weight of LMA and enabling high‐energy‐density batteries. The HCA/C promotes uniform lithium deposition even under rapid charging (up to 5 mA cm−2) owing to its efficient mixed ion/electron conduction pathways. Thus, the HCA/C demonstrates stable cycling for 200 cycles with a low negative/positive ratio of 1.0 when paired with a LiNi0.8Co0.1Mn0.1O2 cathode (areal capacity of 5.0 mAh cm−2). Furthermore, a stacked pouch‐type full cell using HCA/C realizes a high energy density of 344 Wh kg−1cell/951 Wh L−1cell based on the total mass of the cell, exceeding previously reported pouch‐type full cells. This work paves the way for LMA development in high‐energy‐density Li metal batteries. Lithium metal anode should satisfy significant requirements related to fast‐charging feasibility and high‐energy‐density battery design. The hyperporous/hybrid conductive electrode induces simultaneous lithium deposition and facile lithium densification kinetics at fast current density. Besides, carbon‐based ultra‐light architecture realizes dramatic weight reduction of lithium metal anode, compared with a typical metal current collector to effectively achieve high gravimetric energy density.