Hierarchical MXene–Carbon Nanotube Architectures for High‐Stability Silicon Oxide Anodes

Silicon and silicon oxide (SiO x ) are promising anode materials for next‐generation lithium‐ion batteries (LIBs), but their practical use is hindered by severe volume expansion and poor cycling stability. 1D carbon nanotubes (CNTs) and 2D MXenes (Ti 3 C 2 ) both have excellent mechanical and electrical properties, which can be combined to create a more electrically‐interconnected structure with improved mechanical properties. Here, a novel MXene–CNT hierarchical framework synthesized via molecularly driven assembly and crosslinking is reported, enabling electrically interconnected and mechanically reinforced Si/SiO x /C composite anodes. The CNTs bridge the MXene flakes to form a robust conductive network, while the MXene surface chemistry facilitates uniform SiO x /C coating and SEI formation. This architecture significantly suppresses volume expansion (50% after 280 cycles), enhances Li + transport, and stabilizes the SEI layer. As a result, the anode delivers a high initial capacity of 886 mAh g −1 at 200 mA g −1 , retaining 500 mAh g −1 after 280 cycles. In full‐cell configurations with NMC111 cathodes, the CNTMX anode maintains 70% capacity after 500 cycles. These findings demonstrate a scalable strategy for integrating MXene and CNTs to unlock the full potential of silicon‐based anodes in high‐performance LIBs.