Ordered　Pt　alloy　electrocatalysts　supported　on　carbon　nanomaterials　have　attracted　widespread　attention,　especially　for　the　oxygen　reduction　reaction　(ORR),　due　to　the　catalytic　performance　derived　from　their　unique　electronic　and　geometric　structures.　However,　it　is　still　urgent　to　fabricate　uniform　and　structurally　ordered　Pt　alloy　electrocatalysts　based　on　simple　methods.　Herein,　a　two-step　direct　annealing　method　was　applied　to　synthesize　uniform　and　ordered　PtFe　alloy　nanoparticles　loaded　on　single-wall　carbon　nanohorns　(SWCNHs)　under　the　protection　of　a　thin　N-doped　carbon　(NC)　shell,　which　was　in　situ　generated　from　the　polymerization　and　pyrolysis　of　a　small　organic　ligand,　namely,　aniline,　during　the　first　annealing　treatment.　After　the　second　annealing　treatment　in　a　H2　atmosphere　for　9　h,　the　obtained　sample,　denoted　as　PtFe@NC/SWCNHs(H2-9h),　exhibited　uniform　and　ordered　PtFe　nanoparticles　with　a　face-centered　tetragonal　(fct)　structure　(ordered　degree:　＞80%,　mean　size:　∼5.2　nm)　on　the　graphitic　SWCNH　support.　Without　removing　the　NC　shell,　the　PtFe@NC/SWCNHs(H2-9h)　sample　showed　mass　activity　(1.53　A/mgPt　at　0.9　V)　and　specific　activity　(3.61　mA/cm2　at　0.9　V)　toward　the　ORR　due　to　the　enhanced　electronic　interaction　derived　from　the　ordered　fct-PtFe　structure.　Importantly,　it　still　retained　high　catalytic　activity　after　a　long-term　stability　test,　mainly　owing　to　the　ordered　fct-PtFe　structure　and　the　protection　of　the　NC　shell,　which　provides　strong　resistance　toward　the　Fe　leaching　and　nanoparticle　aggregation,　respectively.　The　presented　strategy　is　generalized　to　fabricate　different　ordered　PtM　or　Pt3M　(M　=　Fe/Co)　alloy　electrocatalysts.　©　2021　American　Chemical　Society.