Hybrid　MoS2/C　nanostructures　have　shown　great　promise　as　an　ideal　anode　for　lithium-ion　batteries　(LIBs)　owing　to　the　improved　conductivity　and　electrochemical　performance.　Nevertheless,　if　only　one　side　of　MoS2　particles　is　covered　by　conductive　carbon　layer,　other　exposed　side　is　still　low　conductivity.　Meanwhile,　the　structure　of　electrodes　is　relatively　not　robust.　Herein,　an　effective　structural　engineering　strategy　has　been　proposed　for　achieving　a　new　type　of　polypyrrole-derived　carbon　nanotubes@MoS2@carbon　(PCN@MoS2@C)　sandwiched　architecture　via　a　facile　one-pot　hydrothermal　process.　When　utilized　as　anodes　for　lithium　storage,　the　resulting　MoS2/C　hybrid　exhibits　a　large　specific　capacity　of　1079　mA　h　g(-1)　at　0.1　A　g(-1)　and　high　coulombic　efficiency　of　above　99.0%　over　200　cycles,　showing　a　superior　cycling　stability　and　reversibility.　The　density　functional　theory　(DFT)　calculations　further　demonstrate　that　ultrathin　MoS2　nanosheets　with　an　expanded　interlayer　distance　of　0.98　nm　have　more　accessible　space,　lower　transfer　resistance,　and　faster　diffusion　kinetics　of　Li　ions.　The　great　improvement　in　electrochemical　properties　is　mainly　ascribed　to　the　design　of　peculiar　hybrid　architecture,　and　the　collaborative　effect　between　active　MoS2　nanosheets　and　two　different　conductive　carbon　layers.　This　work　sheds　a　new　light　on　the　rational　design　of　advanced　electrode　materials　with　boosted　performance　and　stable　structural　stability.