Achieving　high　catalytic　activity　with　a　minimum　amount　of　platinum　(Pt)　is　crucial　for　accelerating　the　cathodic　hydrogen　evolution　reaction　(HER)　in　proton　exchange　membrane　(PEM)　water　electrolysis,　yet　it　remains　a　significant　challenge.　Herein,　a　directed　dual-charge　pumping　strategy　to　tune　the　d-orbital　electronic　distribution　of　Pt　nanoclusters　for　efficient　HER　catalysis　is　proposed.　Theoretical　analysis　reveals　that　the　ligand　effect　and　electronic　metal-support　interactions　(EMSI)　create　an　effective　directional　electron　transfer　channel　for　the　d-orbital　electrons　of　Pt,　which　in　turn　optimizes　the　binding　strength　to　H*,　thereby　significantly　enhancing　HER　efficiency　of　the　Pt　site.　Experimentally,　this　directed　dual-charge　pumping　strategy　is　validated　by　elaborating　Sb-doped　SnO2　(ATO)　supported　Fe-doped　PtSn　heterostructure　catalysts　(Fe-PtSn/ATO).　The　synthesized　3%Fe-PtSn/ATO　catalysts　exhibit　lower　overpotential　(requiring　only　10.5 mV　to　reach　a　current　density　of　10 mA cm−2),　higher　mass　activity　(28.6　times　higher　than　commercial　20 wt.%　Pt/C),　and　stability　in　the　HER　process　in　acidic　media.　This　innovative　strategy　presents　a　promising　pathway　for　the　development　of　highly　efficient　HER　catalysts　with　low　Pt　loading.　©　2023　Wiley-VCH　GmbH.