Platinum　(Pt),　as　a　commonly　used　electrocatalyst　in　direct　methanol　fuel　cells　(DMFCs),　suffers　from　sluggish　kinetics　of　both　the　methanol　oxidation　reaction　(MOR)　and　oxygen　reduction　reaction　(ORR).　Geometric　engineering　has　been　proven　effective　for　improving　the　MOR　and　ORR　activities.　Thus,　by　modulating　the　Pt　precursor　and　poly(vinylpyrrolidone)　(PVP)　dosages,　different　porous　PtCu　nanotubes　constructed　by　hollow　nanospheres,　solid　alloy,　and　Pt-rich　skinned　nanoparticles,　respectively,　are　successfully　synthesized.　Among　them,　the　solid　PtCu　alloy　nanoparticle　coherent　nanotubes　exhibit　the　specific　activity　9.42　times　higher　than　Pt/C　toward　MOR,　while　the　hollow　PtCu　alloy　nanosphere　coherent　nanotubes　show　the　specific　activity　4.85　times　higher　than　Pt/C　toward　ORR.　The　different　Pt:Cu　ratios　of　hollow　nanospheres,　solid　alloy,　and　Pt-rich　skinned　nanoparticles　cause　the　differences　in　electron　transfer　from　Cu　to　Pt　as　well　as　electronic　structures　of　Pt.　As　a　result,　the　binding　energies　of　intermediates　can　be　regulated,　leading　to　the　enhancement　in　MOR　and　ORR.　©　2022　Wiley-VCH　GmbH.