Solvent‐Free Roll‐Pressed Sandwiched Li Anode With Dual‐Sided Cu Nanowire Networks for High‐Energy Lithium Metal Batteries

ABSTRACT Li metal anodes are promising for next‐generation high‐energy batteries, but their practical use is hindered by dendritic Li growth, unstable interfaces, and large volume fluctuations. Herein, we report a bidirectional sandwich‐structured Li metal anode (SLA) fabricated through a solvent‐free rolling and pressing strategy. The SLA integrates an ultrathin Li layer with thermally stable 3D Cu nanowire networks on both sides, forming a lightweight, flexible, and mechanically robust electrode. The interconnected Cu nanowire framework provides continuous electron pathways, homogenizes current distribution, and accommodates Li volume changes, thereby guiding uniform Li deposition and stripping within the electrode interior. Benefiting from this design, the SLA achieves a high Coulombic efficiency of 98.73% over 250 cycles at 1 mA cm −2 and 1 mAh cm −2 , while symmetric cells operate stably for over 1350 h with low polarization. Full cells paired with high‐loading NCM811 cathodes deliver excellent cycling stability and rate capability. For a 4‐layer stacked pouch cell, the SLA‐based system delivers a gravimetric energy density of 279.11 Wh kg −1 and a volumetric energy density of 470.52 Wh L −1 , outperforming the PLA counterpart. This work provides a simple strategy for advancing stable Li metal anodes and high‐energy‐density Li metal batteries.