Curved Nanographene–Graphite Hybrid Anodes with Sequential Li + Insertion for Fast‐Charging and Long‐Life Li‐Ion Batteries

Abstract Graphite remains the most widely used anode material for lithium‐ion batteries (LIBs). However, improvements are essential to meet the demand for high‐performance anodes in full‐cell configurations. Here, the synergistic electrochemical performance of a curved nanographene–graphite hybrid anode composed of mesocarbon microbeads (MCMB) is investigated, and Cl‐substituted contorted hexabenzocoronene (Cl‐cHBC), designed to improve the specific capacity, rate capability, and cycling stability. The optimized 1:1 blend forms a homogeneous morphology, in which sphere‐like MCMB particles are uniformly embedded within needle‐like Cl‐cHBC crystals without macrophase separation. This architecture enables sequential Li‐ion insertion and leads to a synergistic improvement in the electrochemical performance. In a half‐cell, the hybrid anode achieves 100 mAh g −1 at 4 A g −1 , outperforming the pristine MCMB graphite (≈20 mAh g −1 at 4 A g −1 ). In full‐cells paired with a single‐crystal LiNi 1‐y‐z Co y Mn z O 2 811 cathode, it shows exceptional rate capability (≈100 mAh g −1 at 5 C) and stability (70% capacity retention after 1000 cycles at 5 C). Furthermore, a pouch cell incorporating the hybrid anode delivers 115 mAh g −1 at 1 C and stable performance over 2100 cycles with a Coulombic efficiency of 99%. These results demonstrate the practical potential of sequential Li‐ion insertion into Cl‐cHBC/MCMB composites for high‐performance LIB applications.