Ammonia-fueled　solid　oxide　fuel　cell　(NH3-SOFC)　presents　a　synergistic　avenue　towards　renewable　energy　yet　it　remains　challenging　due　to　the　sluggish　kinetics　of　NH3　electro-oxidation　in　traditional　Nickel–yttria　stabilized　zirconia　(Ni–YSZ).　Herein,　we　employ　La1-xSrxFeO3-δ　(LSF)　via　Sr2+　substitution　strategy　in　classical　LaFeO3　perovskite　as　anode,　aiming　to　boost　energy　power　generation　for　NH3-SOFC.　Interestingly,　the　structure　of　LSF　transforms　from　single　perovskite　to　Ruddlesden-Popper　(R-P)　layered　perovskite　with　exsolution　of　Fe　nanoparticles　while　no　phase　change　in　LaFeO3　is　found　under　reducing　conditions.　Such　a　Sr-induced　structural　evolution　can　throttle　the　H2　adsorption　capacity　to　retard　the　“hydrogen　poisoning”　behavior　and　endow　LSF　with　medium-strong　basic　sites,　facilitating　efficient　recombination　of　N　atoms　into　N2　molecules　for　NH3　electro-oxidation.　The　R-P　structure　perovskite　LSF　induces　changes　in　charge　density,　facilitating　the　accommodation　of　abundant　oxygen　vacancies.　The　release　of　active　Fe　nanoparticles　promotes　the　exposure　of　active　sites,　enhancing　electron　transfer　and　resulting　in　high　catalytic　performance　and　excellent　stability.　As　a　result,　the　maximum　power　output　of　LSF　anode　using　NH3　reaches　98　%　of　that　of　H2　and　is　3.7　times　higher　than　that　of　Ni-YSZ.　The　preferential　NH3　oxidation　mechanism　is　proposed　in　view　of　relaxation　time　distribution　as　well　as　Bode　plots.　©　2025