The　poor　conductivity　of　sulfur,　non-uniform　Li2S　deposition,　polysulfide　shuttle　effect,　and　slow　reaction　kinetics　severely　hinder　the　commercialization　of　flexible　lithium‑sulfur　batteries.　Herein,　a　unique　flexible　self-supporting　sulfur　host　featuring　a　dual‑carbon　layer　hierarchical　structure　is　developed,　which　possesses　the　following　roles:　1)　the　inner　three-dimensional　carbon　nanotube　conductive　network　promotes　electron　and　ion　transport,　alleviates　sulfur　volume　expansion,　and　physically　confines　active　materials;　2)　the　outer　carbon　layer　modified　with　CoSe2　nanoparticles　functions　as　a　chemical　adsorption　carrier　and　electrocatalyst,　effectively　anchoring　polysulfide　and　enhancing　their　conversion　kinetics.　The　innovative　design　of　the　dual‑carbon　layer　hierarchical　structure　and　the　“confinement–adsorption–catalysis”　synergistic　effect　enable　uniform　Li2S　deposition　and　significant　enhancement　of　sulfur　cathode　electrochemical　performance.　Consequently,　DC/CoSe2-S　exhibited　a　low　capacity　decay　rate　of　0.07%　per　cycle　over　400　cycles　at　1C,　with　an　average　Coulombic　efficiency　of　99.3%.　Notably,　DC/CoSe2-S　maintained　a　capacity　retention　of　98.4%　at　0.1C　for　100　cycles　with　a　high　sulfur　loading　of　4.0　mg　cm−2　(Electrolyte/Sulfur　=　10　μL　mg−1).　Furthermore,　the　constructed　pouch　cells　(Sulfur　loading　=　4.0　mg　cm−2,　Electrolyte/Sulfur　=　8.6　μL　mg−1)　also　operated　stably　for　50　cycles,　demonstrating　the　promising　potential　for　practical　applications.　This　work　provides　new　insights　into　the　design　of　high-performance　flexible　lithium‑sulfur　batteries.　©　2025　Elsevier　B.V.