Dual Vertically Aligned Electrode‐Inspired High‐Capacity Lithium Batteries

Lithium (Li) dendrite formation and poor Li(+) transport kinetics under high‐charging current densities and capacities inhibit the capabilities of Li metal batteries (LMBs). This study proposes a 3D conductive multichannel carbon framework (MCF) with homogeneously distributed vertical graphene nanowalls (VGWs@MCF) as a multifunctional host to efficiently regulate Li deposition and accelerate Li(+) transport. A novel electrode for both Li|VGWs@MCF anode and LFP|VGWs@MCF (NCM(811)|VGWs@MCF) cathode is designed and fabricated using a dual vertically aligned architecture. This unique hierarchical structure provides ultrafast, continuous, and smooth electron transport channels; furthermore, it furnishes outstanding mechanical strength to support massive Li deposition at ultrahigh rates. As a result, the Li|VGWs@MCF anode exhibits outstanding cycling stability at ultrahigh currents and capacities (1000 h at 10 mA cm(–2) and 10 mAh cm(–2), and 1000 h at 30 mA cm(–2) and 60 mAh cm(–2)). Moreover, full cells made of such 3D anodes and freestanding LFP|VGWs@MCF (NCM(811)|VGWs@MCF) cathodes with conspicuous mass loading (45 mg cm(–2) for LFP and 35 mg cm(–2) for NCM(811)) demonstrate excellent areal capacities (6.98 mAh cm(–2) for LFP and 5.6 mAh cm(–2) for NCM(811)). This strategy proposes a promising direction for the development of high‐energy‐density practical Li batteries that combine safety, performance, and sustainability.