Metal–organic　frameworks　(MOFs)　have　been　extensively　studied　due　to　their　porous　structures　and　large　specific　surface　areas.　Its　unique　combination　of　central　metal　and　organic　ligand　has　become　a　common　precursor　for　the　synthesis　of　metal　phosphides,　selenides,　oxides,　and　sulfides.　However,　the　carbonaceous　structure　derived　from　some　MOF　materials　is　still　not　enough　to　perfectly　alleviate　the　negative　impact　of　the　volume　change　of　metal　sulfides.　Herein,　bimetallic　MOF　(Zn-Co-ZIF)　is　used　as　a　precursor,　coated　with　dopamine　hydrochloride,　and　then　calcined　and　gas-phase　vulcanized　to　prepare　ZnS/CoS2-C@NC　with　a　double-carbon-layer　core–shell　structure.　The　existence　of　the　two　carbonaceous　structures　can　not　only　improve　the　electron　transport　ability,　but　also　play　an　important　role　in　alleviating　the　volume　expansion　caused　by　metal　sulfides　during　repeated　charging　and　discharging.　Due　to　its　stable　carbon　layer　structure,　ZnS/CoS2-C@NC　has　a　higher　specific　capacity　(1175.4　mAh　g−1　in　lithium-ion　batteries　(LIBs)　and　430.9　mAh　g−1　in　sodium-ion　batteries　after　100　cycles　at　a　current　density　of　0.2　A　g−1　respectively)　and　excellent　rate　capability　(338.2　mAh　g−1　specific　capacity　maintained　after　2000　cycles　at　a　current　density　of　5　A　g−1　in　LIBs).　©　2023　Wiley-VCH　GmbH.