In　this　work,　a　surface　engineering　strategy　has　been　developed　to　implant　atomic　Ni　mostly　enriched　in　1　nm　thickness　of　MoS2　nanosheets,　and　suppresses　the　segregation　of　undesired　NiSx.　Notably,　this　structural　regulation　not　only　creates　additional　edges　exposed　at　the　inert　basal　plane　of　MoS2　nanosheets,　but　also　increases　the　catalytic　ability　of　edge　sites　by　forming　dominant　NiMoS　phase.　As　such,　a　low　overpotential　of　95　mV　is　achieved　to　deliver　a　current　density　of　10　mA　cm−2,　which　is　242　mV　decrease　than　unmodified　MoS2,　together　with　86.5%　preservation　of　initial　capacity　after　100　h　test.　Theoretical　calculations　further　identify　the　activated　catalytic　sites　both　in　Mo-edge　and　S-edge,　and　the　specific　atomic　configurations　enable　the　synergistic　effect　to　optimize　the　adsorption-desorption　of　H∗,　and　is　responsible　for　the　remarkably　improved　hydrogen　evolution　reaction　(HER)　activity.　©　2023　Hydrogen　Energy　Publications　LLC