The large-scale deployment of a terawatt-level proton exchange membrane water electrolyzer (PEMWE) requires highly active and durable platinum (Pt)-based catalysts for efficient hydrogen evolution reaction (HER). However, conventional Pt-based catalysts suffer from high costs, resource scarcity, and stability challenges in acidic environments. Here, we apply a solvent-free strategy to precisely functionalize single-walled carbon nanotubes, enabling the covalent anchoring of Pt nanoparticles. The electron-donating amino functional group exhibits dual roles in Pt modification by simultaneously regulating the particle size distribution of Pt nanoparticles and tailoring their electronic structure via strong Pt–support interactions. As a result, a PEMWE incorporating this catalyst achieves a low cell voltage of 2.1 V with an impressive mass activity of 3.98 A mg Pt –1 while demonstrating robust durability at 500 mA cm –2 during continuous operation for 60 h. These findings highlight the potential of functional group engineering in designing next-generation HER catalysts for scalable hydrogen production.