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　N-2-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　N-2　activation　energy　via　strong　electron　＂sigma-donation　and　pi-backdonation＂　between　Ru　and　N-2　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　N(2)H(4)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　mmol(NH3)　g(-1)　h(-1)　at　360　degrees　C　and　3　MPa)　among　the　Ru　or　Co-based　catalysts　ever　reported.