Simultaneously　achieving　a　low　activation　barrier　with　weak　binding　of　intermediates　on　a　heterogeneous　catalyst　for　the　enhancement　of　catalytic　performance　under　mild　conditions　remains　a　great　challenge,　especially　for　N2-to-NH3　conversion.　Herein,　for　the　first　time,　we　report　a　new　strategy　via　integrating　vacuum-freeze-drying　and　high-temperature　pyrolysis　technologies　to　design　atomically　dispersed　Co　deposits　onto　the　surface　of　Ru　tiny　subnanoclusters　(TCs).　The　special　structure　of　this　catalyst　can　generate　a　spatial　effect　and　induce　strong　interelectronic　interactions　between　Ru　and　Co.　The　outcome　is　simultaneous　generation　of　the　high-surface-unoccupied　Co　3d　charge　and　obvious　upshifting　of　the　Ru　d-band　center.　With　that,　there　is　lowering　of　N2　activation　energy　via　strong　electron　＇σ-donation　and　π-backdonation＇between　Ru　and　N2　molecules.　More　importantly,　our　studies　demonstrate　that　an　appropriate　Ru　structure　with　tiny　subnanoclusters　rather　than　single　Ru　atoms　or　large　Ru　clusters　could　enable　the　repulsion　to　adsorption　of　the　N-containing　intermediates　on　the　catalyst　surface,　resulting　in　weakening　of　the　binding　of　NH3　and　N2H4　intermediates　on　the　Co1Ru　TC　catalyst　surface.　In　such　a　case,　the　scaling　relation　over　Co1Ru　TCs　in　NH3　synthesis　was　decoupled,　and　the　developed　Ba-promoted　Co1Ru　TC　catalyst　shows　the　highest　NH3　synthesis　rate　(up　to　21.90　mmolNH3　g-1　h-1　at　360　°C　and　3　MPa)　among　the　Ru　or　Co-based　catalysts　ever　reported.　©　2021　American　Chemical　Society.