Anchoring <scp> MoS ₂ </scp> Petal‐Like Nanosheets on Coal‐Based Carbon Nanofibers by Surface Bonding Enable Li ⁺ /Na ⁺ Batteries to Achieve Fast‐Charging Capabilities

The unique layered architecture and redox‐active nature of two‐dimensional molybdenum disulfide (2D MoS 2 ) nanosheets have motivated their widespread utilization as anode materials in rechargeable lithium‐ion (LIBs) and sodium‐ion (SIBs) batteries. However, their low electrical conductivity, significant volume changes, and rapid capacity fading lead to poor cycling performance. Herein, MoS 2 nanosheet‐decorated coal‐based carbon nanofibers (MoS 2 @CCNFs) were synthesized through electrostatic spinning and solvothermal methods. Experimental results and density functional theory (DFT) calculations reveal that the C‐S/C‐O‐S heterointerface‐mediated architecture significantly enhances the interfacial transport kinetics of Li + /Na + , Simultaneously, coal‐derived carbon reinforcement improves the mechanical robustness of nanofibers, thereby optimizing both electronic conductivity and structural stability of the composite electrode. Furthermore, the mechanism of Li + /Na + storage was further investigated through in‐situ X‐ray diffraction (XRD). As anticipated, the MoS 2 @CCNFs electrode delivered outstanding cycling stability, retaining a high capacity of 350.8 mAh g −1 after 2000 cycles at 10.0 A g −1 in LIBs. Similarly, for SIBs, the electrode exhibited a remarkable capacity of 400.3 mAh g −1 after 1000 cycles at 5.0 A g −1 . In full‐cell configurations, the MoS 2 @CCNFs||LiCoO 2 and MoS 2 @CCNFs||NaFePO 4 systems demonstrated specific capacities of 84.3 mAh g −1 and 64.3 mAh g −1 , respectively, following 120 cycles at 0.2 C rate, demonstrating excellent cycling stability in both battery systems.