Recently,　the　rational　design　of　stable　and　efficient　electrocatalysts　remains　a　major　challenge　for　the　hydrogen　evolution　reaction　(HER)　under　alkaline　conditions.　Herein,　using　zeolitic　imidazolate　framework-67　(ZIF-67)　as　a　template,　we　successively　deposited　ammonium　molybdate　and　wrapped　the　complex　of　trithiocyanuric　acid　(TCA)　and　Cu.　Through　one-step　high-temperature　sulfidation,　the　CoS@MoS2/Cu2S@NC　catalyst　with　porous,　ball-in-ball,　and　yolk-shell　structures　was　successfully　synthesized.　This　unique　structure　can　effectively　increase　the　specific　surface　area,　enhance　mass　transport,　and　expose　more　active　sites.　Additionally,　the　synergistic　effect　between　N-doped　C　and　various　active　components　such　as　metal　sulfides　enhances　the　electrochemical　activity　of　the　catalyst.　Based　on　these　advantages,　CoS@MoS2/Cu2S@NC　requires　only　149,　175,　and　199　mV　overpotentials　to　achieve　a　current　density　of　10　mA　cm−2　in　alkaline　water,　simulated　alkaline　seawater,　and　alkaline　seawater,　separately,　accompanied　by　low　Tafel　slopes　of　76.8,　74.7,　and　87.3　mV·dec−1.　Furthermore,　2000　cycles　of　cyclic　voltammetry　(CV)　and　a　100-h　durability　test　demonstrate　its　excellent　catalytic　stability.　This　work　offers　a　strategy　for　designing　transition　metal　sulfide　catalysts　with　high　catalytic　activity　and　sustainability.　©　2025　Hydrogen　Energy　Publications　LLC