With　the　exceptional　merits　of　high　energy　density,　low　cost,　and　environmental　friendliness,　lithium-sulfur　batteries　are　considered　to　be　one　of　the　most　promising　next-generation　flexible　rechargeable　batteries.　However,　the　notorious　“shuttle　effect”　has　seriously　hindered　their　practical　applications.　Herein,　a　strategy　for　designing　multi-functional　bilayer　carbon　structures　is　proposed,　specifically,　by　employing　a　micrometer-thick　graphene　nanoflowers　(GF)　layer　to　encapsulate　a　micrometer-scale　hybrid　network　skeleton　composed　of　metallic　Co　and　carbon　nanotubes　(CNT)　as　a　flexible　sulfur　cathode　host　(Co/CNT@GF).　Beneficial　from　the　merits　of　chemical　adsorption,　electrocatalysis　and　volume　expansion　mitigation　from　the　internal　skeleton　as　well　as　the　micrometer-level　physical　domain　confinement　by　the　external　GF　layer,　the　developed　host　could　chemically　trap,　electrochemically　catalyze,　physically　block　and　storage　the　lithium　polysulfides.　Due　to　the　synergistic　effect　of　these　functions,　the　Co/CNT@GF-S　delivers　a　superior　discharge　capacity　of　799　mAh　g−1　with　a　decay　rate　as　low　as　0.08　%　per　cycle　after　400　cycles　at　1　C.　Even　at　a　high　sulfur　loading　of　8.16　mg　cm−2,　the　average　discharge　capacity　is　as　high　as　5.05　mAh　cm−2　in　100　cycles.　This　work　does　not　only　contribute　to　the　rational　design　of　multi-functional　bilayer　structures　but　also　offers　a　novel　design　method　for　the　commercialization　of　flexible　lithium-sulfur　batteries　with　high-energy–density.　©　2022　Elsevier　B.V.