The　single　atom　catalysts　(SACs)　show　immense　promise　as　catalytic　materials.　By　doping　the　single　atoms　(SAs)　of　precious　metals　onto　substrates,　the　atomic　utilization　of　these　metals　can　be　maximized,　thereby　reducing　catalyst　costs.　The　electronic　structure　of　precious　metal　SAs　is　significantly　influenced　by　compositions　of　doped　substrates.　Therefore,　optimizing　the　electronic　structure　through　appropriate　doping　of　substrates　can　further　enhance　catalytic　activity.　Here,　Pt　single　atoms　(Pt　SAs)　are　doped　onto　transition　metal　sulfide　substrate　NiS2　(Pt　SAs-NiS2)　and　phosphide　substrate　Ni2P　(Pt　SAs-Ni2P)　to　design　and　prepare　catalysts.　Compared　to　the　Pt　SAs-NiS2　catalyst,　the　Pt　SAs-Ni2P　catalyst　exhibits　better　hydrogen　evolution　catalytic　performance　and　stability.　Under　1　M　KOH　conditions,　the　hydrogen　evolution　mass　activity　current　density　of　the　Pt　SAs-Ni2P　catalyst　reaches　0.225　A　mgPt(-1)　at　50　mV,　which　is　33　times　higher　than　that　of　commercial　Pt/C　catalysts.　It　requires　only　44.9　mV　to　achieve　a　current　density　of　10　mA　cm(-2).　In　contrast,　for　the　Pt　SAs-NiS2　catalyst,　the　hydrogen　evolution　mass　activity　current　density　is　0.178　A　mgPt(-1),　requiring　77.8　mV　to　achieve　a　current　density　of　10　mA　cm(-2).　Theoretical　calculations　indicate　that　in　Pt　SAs-Ni2P,　the　interaction　between　Pt　SAs　and　the　Ni2P　substrate　causes　the　Pt　d-band　center　to　shift　downward,　enhancing　the　H2O　desorption　and　providing　optimal　H　binding　sites.　Additionally,　the　hollow　octahedral　morphology　of　Ni2P　provides　a　larger　surface　area,　exposing　more　reactive　sites　and　improving　reaction　kinetics.　This　study　presents　an　effective　pathway　for　preparing　high-performance　hydrogen　evolution　electrocatalysts　by　selecting　appropriate　doped　substrates　to　control　the　electronic　structure　of　Pt　SAs.