[en] High lithium storage capacity and high conductivity of the LIB anode materials are extremely desirable for lithium-ion batteries (LIBs). Herein, the article demonstrated the method of embedding single or few layers 2D MoS₂ into e-spun carbon nanofibers (MS-CNFs) to improve the electrochemical behavior of lithium anode materials. As demonstrated by various microscopic and spectroscopic analyses, MS-CNFs exhibited well-aligned morphology with uniform diameter of 330–360 nm. The roughness surface of MS-CNFs is favorable to shorten ion diffusion pathway and decrease the charge transfer resistance. Moreover, MS-CNFs hybrids exhibit a higher specific capacity of 1172 mAh g⁻¹ with the good rate capability (97.3%) and cycle stability (86.4%) than pristine PAN based carbon nanofibers (p-CNFs) and 2D MoS₂ due to the synergistic effect of pseudocapacitive material MoS₂ and roughness morphology of CNFs. It is anticipated to exploit surface modification of MoS₂ nanosheets and MoS₂-based composites with high performances. - Highlights: • 2D MoS₂-decorated Carbon Nanofibers (MS-CNFs) is prepared via Electron-Spun. • The charge transfer pathway is shorted by the roughness surface of MS-CNFs. • The MS-CNFs hybrids LIBs anode exhibits high reversible capacity and good stability.