Developing　efficient　and　robust　catalysts　for　hydrogen　production　by　ammonia　decomposition　is　of　importance　towards　the　＂zero-carbon＂　economy.　Herein,　a　series　of　B-site　Ni-　and　Co-doped　A-site-deficient　SrTiO3　perovskite　(Sr0.9Ti0.8Ni0.1Co0.1O3-delta,　STNC)　with　the　in　situ　exsolution　of　NiCo　nano-alloys　were　fabricated　under　reducing　atmosphere.　The　Ni-Co/STO　(SrTiO3)　catalyst　derived　from　STNC　shows　much　higher　activity　for　ammonia　decomposition　than　those　Ni　and　Ni-Co　based　catalysts　fabricated　by　impregnation.　The　STNC　derived　sample　can　produce　32.6　mmol　gcat-1　&　sdot;min-　1　hydrogen　at　600　degrees　C,　2.2　and　1.9　fold　higher　than　those　of　Ni/STO　and　Ni-Co/STO.　Furthermore,　the　synthesis　methods　including　the　Pechini,　hydrothermal　and　ball　milling　methods　were　investigated　for　the　preparation　of　the　exsoluted　Ni-Co　catalysts　toward　ammonia　decomposition.　The　STNC-HT　catalyst　by　hydrothermaldemonstrated　an　excellent　performance　and　reached　70%　and　a　near　equilibrium　conversion　of　ammonia　under　600　and　650　degrees　C　with　a　WHSV　of　30,000　mL　gcat　between　structure　and　performance　was　further　studied　by　a　series　of　characterizations.　In　addition,　the　STNC-HT　catalyst　was　employed　in　the　direct　ammonia　solid　oxide　fuel　cells,　in　which　the　performance　is　closely　related　to　the　ammonia　decomposition　activity,　and　shows　a　satisfying　power　density　of　99.3　mW　cm-　2.　Generally,　we　identified　an　approach　to　engineer　catalysts　with　enhanced　activity　for　the　ammonia　utilization　as　energy　vectors　in　our　work.