The　commercial　application　of　lithium-sulfur　batteries　is　severely　hampered　by　polysulfide　shuttle　effects,　sluggish　redox　kinetics,　and　uncontrollable　lithium　dendrite　growth.　Herein,　a　unique　Ni-doped　CoSe2　nanoparticle　decorated　bilayer　carbon　(Ni-CoSe2/BC)　structure　is　synthesized　for　both　the　sulfur　cathode　and　lithium　anode,　which　introduces　bi-functionalities　including　)　the　internal　carbon　conductive　network　skeleton　of　carbon　nanotubes　is　capable　of　physically　confining,　storing,　and　alleviating　volume　expansion　of　sulfur;　and　)　Ni-CoSe2　nanoparticles　decorated　on　the　external　carbon　nanoarrays　contribute　to　efficient　chemical　anchoring　and　accelerated　polysulfide　conversion　for　the　cathode,　and　serve　as　lithiophilic　sites　to　induce　homogeneous　lithium　deposition　for　the　anode.　As　a　result,　Ni-CoSe2/BC　effectively　inhibits　the　shuttle　effect　and　induces　dendrite-free　lithium　deposition.　The　Ni-CoSe2/BC-S　delivers　a　high　discharge　specific　capacity　of　806　mAh　g−1　after　400　cycles　at　1　C,　with　a　low　capacity　decay　rate　of　0.07%　per　cycle.　Moreover,　the　Ni-CoSe2/BC-Li　exhibits　an　impressively　long　cycle　life　of　2000　h　at　10　mA　cm−2/10　mAh　cm−2.　Notably,　the　lithium-sulfur　full　cell　assembled　with　Ni-CoSe2/BC　as　universal　hosts　for　both　anode　and　cathode　possesses　an　average　discharge　capacity　of　6.07　mAh　cm−2　in　50　cycles　(Sulfur　loading=12.8　mg　cm−2,　Electrolyte/Sulfur=7.8　μL　mg−1,　and　Negative/Positive=1.56).　This　work　provides　novel　structural　design　and　mechanism　insights　for　the　practical　application　of　lithium-sulfur　batteries.　©　2023　Elsevier　B.V.