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.