<p>Rationally designing the surface structure with desirable facets has been demonstrated as an effective approach to regulating the catalytic activity and anti-CO poisoning capability of Pd-based catalysts for methanol oxidation reaction (MOR). However, the synthesis of Pd-based alloy with high-index facets to further improve Pd utilization remains a fundamental challenge. Herein, a simple solvothermal method was proposed to synthesize the jagged PtPdTe nanotubes (NTs) with abundant zigzag atomic steps on their surfaces. These zigzag facets are more favorable for both the adsorption of OH and the desorption of CO during MOR. Compared with the smooth PtPdTe NTs, the jagged PtPdTe NTs exhibit an enhanced mass activity of 4201.6 mA mg⁻¹ and specific activity of 4.12 mA cm⁻², which are 6.7 and 3.2 times higher than those of commercial Pd/C catalysts, respectively. This work not only advances the understanding of surface engineering in catalysis but also extends the novel design of highly efficient and durable Pd-based catalysts for fuel cells.</p>