Platinum　is　the　best　electrocatalyst　for　the　hydrogen　evolution　reaction　(HER).　Here,　we　demonstrate　that　by　contact　electrification　of　Pt　nanoparticle　satellites　on　a　gold　or　silver　core,　the　Fermi　level　of　Pt　can　be　tuned.　The　electronic　properties　of　Pt　in　such　hybrid　nanocatalysts　were　experimentally　characterized　by　X-ray　photoelectron　spectroscopy　(XPS)　and　surface-enhanced　Raman　scattering　(SERS)　with　the　probe　molecule　2,6-dimethyl　phenyl　isocyanide　(2,6-DMPI).　Our　experimental　findings　are　corroborated　by　a　hybridization　model　and　density　functional　theory　(DFT)　calculations.　Finally,　we　demonstrate　that　tuning　of　the　Fermi　level　of　Pt　results　in　reduced　or　increased　overpotentials　in　water　splitting.　©　2023　The　Authors.　Angewandte　Chemie　International　Edition　published　by　Wiley-VCH　GmbH.