Controllable Particle Packing via Scalable Layer‐by‐Layer Assembly of Anode Particles for Fast‐Charging Lithium‐Ion Batteries

Particle packing in battery electrodes is pivotal to the fast‐charging performance of lithium‐ion batteries (LIBs). However, precise control of particle packing structure remains a major challenge in electrode fabrication, primarily owing to the absence of robust interfacial bonding between micron‐scale particles. Herein, we propose a novel layer‐by‐layer single‐layer particle assembly technique to fabricate electrodes with well‐defined particle packing structures. Using this approach, we prepared a 12‐meter‐long graphite (Gr)/hard carbon (HC) hybrid anode featuring a body‐centered cubic (BCC)‐like structure, which maximizes intimate Gr/HC contact interfaces and facilitates solid‐state Li + transport. Coupled with LiFePO 4 (LFP) cathodes, the as‐fabricated anode exhibits a high‐capacity retention of 80.7% after 1650 cycles at 4C. From an electrode design standpoint, this controllable particle‐packing strategy paves the way for a universal framework for developing sustainable, long‐cycling, and fast‐charging electrodes, potentially applicable to many types of battery anodes and cathodes.