The　development　of　high-performance　electrocatalysts　for　hydrogen　evolution　reaction　(HER)　in　different　pH　conditions　is　pivotal　in　producing　green　hydrogen,　but　remains　challenging.　Herein,　we　regulate　the　p-d　orbitals　hybridization　between　B　and　Pt　for　effective　and　durable　HER　at　all　pH　ranges　by　controlling　the　inserted　B　atom.　Consequently,　the　optimized　B-doped　Pt　catalysts　with　20　at.%　B　content　(Pt80B20/C)　has　the　highest　HER　performance,　with　only　7　mV　overpotential　in　acidic　conditions,　37　mV　in　alkaline　media,　and　47　mV　in　neutral　media,　more　remarkably,　have　negligible　attenuation　during　electrolysis　up　to　100　h,　which　is　superior　to　commercial　Pt/C　catalysts.　Theoretical　calculations　revealed　that　by　inserting　appropriate　B　atoms　in　the　interstitial　vacancies　of　Pt,　the　electronic　structure　of　Pt　is　suitable　for　providing　appropriate　hydrogen　intermediates　(H*)　adsorption/desorption　strength,　resulting　in　superior　acid　HER　electrocatalyst　performance.　Besides,　a　strong　electronic　interaction　existed　between　Pt　and　inserted-B　atoms　leaving　Pt　sites　in　an　electron　deficiency　state,　which　facilitates　the　bond　cleavage　of　the　H-OH　of　H2O,　hence　accelerating　water　dissociation　and　promoting　neutral/alkaline　HER　dynamics.　©　2025　Elsevier　Inc.