Dual-atom　catalysts　(DACs)　with　paired　active　sites　can　provide　unique　intrinsic　properties　for　heterogeneous　catalysis,　but　the　synergy　of　the　active　centers　remains　to　be　elucidated.　Here,　we　develop　a　high-performance　DAC　with　Zn1Co1　species　anchored　on　nitrogen-doped　carbon　(Zn1Co1/NC)　as　the　dominant　active　site　for　the　propane　dehydrogenation　(PDH)　reaction.　It　exhibits　several　times　higher　turnover　frequency　(TOF)　of　C3H8　conversion　and　enhanced　C3H6　selectivity　compared　to　Zn1/NC　or　Co1/NC　with　only　a　single-atom　site.　Various　experimental　and　theoretical　studies　suggest　that　the　enhanced　PDH　performance　stems　from　the　promoted　activation　of　the　C-H　bond　of　C3H8　triggered　by　the　electronic　interaction　between　Zn1　and　Co1　colligated　by　N　species.　Moreover,　the　dynamic　sinking　of　the　Zn1　site　and　rising　of　the　Co1　site,　together　with　the　steric　effect　of　the　dissociated　H　species　at　the　bridged　N　during　the　PDH　reaction,　provides　a　feasible　channel　for　C3H6　desorption　through　the　more　exposed　Co1　site,　thereby　boosting　the　selectivity.　This　work　provides　a　promising　strategy　for　designing　robust　hetero　DACs　to　simultaneously　increase　activity　and　selectivity　in　the　PDH　reaction.　©　2023　American　Chemical　Society.