Gas diffusion layer (GDL) plays a crucial role in enhancing the protonexchange membrane fuel cell (PEMFC) performance. However, the conventional GDL preparation method is typically complex and expensive, which involves coating carbon paper with polytetrafluoroethylene (PTFE) followed by high-temperature sintering. Herein, we propose a facile and low-cost strategy to fabricate surface-functionalized GDL via covalent bonding interaction with the hydrophobic agent. Benefiting from the favorable chemical grafting with a family of silane coupling agents (perfluorooctyltriethoxysilane, cetyltrimethoxysilane, and 3-aminopropyltriethylsilane), the optimized carbon paper shows high porosity and pore size (average pore diameter: 28.89 μm) as well as the superhydrophobicity (water contact angle: ∼ 150.2°) properties. As a result, the modified GDL with oxidation followed by cetyltrimethoxysilane (O-GDL-C) grafting treatment endows the PEMFC with augmented water and gas permeability, affording a peak power density of 866.4 mW cm −2 . This work paves a new way to construct an efficient GDL for PEMFCs via facile chemical grafting technology.