Enhanced Kinetics and Dual‐Interfacial Stability in High‐Areal‐Loading Electrodes for Lithium Metal Batteries via Crosstalk‐Active Polymer‐Functionalized Carbon Nanotubes

Abstract With the rapid shift toward sustainable energy systems, battery technologies offering high energy densities and long cycle life are critical. Lithium metal batteries (LMBs) are central to achieving high energy storage required by global sustainability efforts, yet their practical deployment faces critical limitations, including dendritic lithium deposition and challenges associated with thick cathode structures. To simultaneously overcome these issues, this research develops a polymer‐functionalized carbon nanotube framework grafted with poly(2‐acrylamido‐2‐methylpropane sulfonic acid), effectively enhancing dispersion, ionic transport, and electrode integrity. A unique cathode–anode crosstalk, arising from the sulfonic acid functional groups, stabilizes lithium interfaces and significantly mitigates dendrite formation, as revealed by computational studies. Advanced characterizations confirm improved Li⁺ kinetics, reduced interfacial resistances, and long‐term cycling stability. Implementing in pouch cells, this strategy achieves a remarkable energy density of 453.2 Wh kg −1 . This holistic approach provides a practical and scalable strategy to overcome key commercial barriers, paving the way for next‐generation LMBs.