The　development　of　earth-rich,　low-cost,　and　high-efficiency　electrocatalysts　toward　alkaline　hydrogen　evolution　reactions　(HERs)　in　the　water　spitting　process　is　extremely　desirable　yet　a　huge　challenge.　In　this　work,　we　report　the　synthesis　of　novel　RuO2/MoS2　electrocatalysts　with　good　conductivity　and　abundant　active　sites　for　efficient　HER　by　uniformly　dispersing　RuO2　nanoparticles　on　MoS2　nanosheets.　Benefitting　from　the　intense　electronic　coupling　effect　endowed　with　interface　modifications,　the　as-prepared　RuO2/MoS2　electrocatalysts　exhibited　superior　performance　for　HER　in　1　M　KOH　with　a　very　low　overpotential　of　36　mV　at　10　mA　cm−2　and　a　small　Tafel　slope　value　of　34.8　mV　dec−1.　Moreover,　the　introduction　of　RuO2　nanoparticles　improved　the　durability　of　the　RuO2/MoS2　electrocatalysts　with　negligible　variation　in　a　20　h　operation.　More　importantly,　the　density　functional　theory　(DFT)　calculations　further　revealed　the　mechanism　of　strong　electronic　interaction　between　RuO2　nanoparticles　and　MoS2　nanosheets,　which　contributes　to　accelerating　the　H2O　dissociation　kinetics　and　optimizing　H　adsorption　Gibbs　free　energy.　This　work　may　provide　a　deeper　understanding　for　designing　efficient　HER　catalysts　through　interface　modification　strategies.　©　2023　The　Royal　Society　of　Chemistry.