Alloying is a general and efficient strategy to boost the catalytic activity of Pt catalysts toward oxygen reduction reaction (ORR) through electronic and geometric effects. Besides, high-index surfaces (HISs) of Pt also exhibit superior ORR activity, mainly originated from low-coordinated step or kink atoms. Thus, a combination of the alloying and HISs would be a promising method to further develop excellent catalysts for ORR. However, simultaneous control of alloy composition and HISs exposure in nanoscale remains challenging.