Al-S　batteries　offer　advantages　such　as　high　energy　density,　low　cost,　and　good　safety.　However,　they　face　challenges　including　poor　sulfur　conductivity,　volume　expansion,　and　slow　kinetics　of　polysulfides,　leading　to　rapid　capacity　decay　and　short　cycle　life.　Therefore,　the　design　of　materials　with　high　conductivity,　capable　of　anchoring　polysulfides,　and　structurally　robust　is　crucial　for　enhancing　the　overall　performance　of　Al-S　batteries.　To　address　these　issues,　we　propose　the　construction　of　a　structurally　stable　graphene-carbon　nanotubes　(CNTs)　covalently　bonded　hybrid　and　a　three-dimensional　(3D)　conductive　framework　catalyzed　by　Co　active　sites.　The　porous　Co,　N-doped　graphene-carbon　nanotubes　(CoN-GC)　hybrid　with　excellent　mechanical　properties　provides　sufficient　space　for　high　sulfur　loading,　alleviating　sulfur　volume　expansion.　Co　plays　a　key　role　in　rapidly　transporting　electrons,　adsorbing,　and　catalyzing　aluminum　polysulfides.　The　Al-S　battery　using　S@CoN-GC　cycles　over　1500　cycles　at　a　current　density　of　300　mA·g−1,　maintaining　a　specific　capacity　of　315　mAh·g−1,　and　retains　278　mAh·g−1　after　2000　cycles.　Additionally,　utilizing　the　outstanding　mechanical　properties　of　CoN-GC,　a　flexible　Al-S　microbattery　was　successfully　fabricated,　maintaining　a　capacity　retention　of　90　%　after　folding　1000　times.　These　research　findings　are　expected　to　accelerate　the　study　of　multivalent　metal-sulfur　batteries　and　their　practical　applications　in　various　scenarios.　©　2024　Elsevier　B.V.