Engineering nanoparticle surfaces driven by various gas atmospheres has attracted intensive attention in the design of efficient electrocatalysts for sustainable energy applications. However, the development of a more facile and efficient in situ engineering strategy under electrochemical testing conditions to achieve surface-reconstruction-induced high performance is significantly lacking. Herein, for the first time, we report in situ high-potential-driven restructuring in ternary AgPdPt aerogels with dilute Pt (AgPd–Ptdilute) during the electrochemical cyclic voltammetry testing for the alkaline formate oxidation reaction (FOR), in which the upper potential limit is ingeniously extended to the Ag redox region. Impressively, the resulting AgPd–Ptdilute aerogel displayed remarkable structural and compositional reconstruction in an alkaline environment. Our comprehensive results revealed that the high-potential cycling induces unique Ag outward diffusion to form an enriched PdPt metallic surface atomically coupled with amorphous Ag2O, which provides more opportunities to expose abundant active sites and induce robust electronic structure modulation. Notably, the surface-restructured AgPd–Ptdilute aerogel achieved record-high activity for FOR when the upper potential limit was extended to 1.3 V, exhibiting an unprecedented 5-fold improvement in activity compared to that of the commercial Pd/C. Moreover, it also offered greatly enhanced electrochemical stability with negligible activity decay after 500 cycles. This work gives a good understanding of surface reconstruction during such a novel high-potential-driven cycling process and opens a new door to designing more efficient electrocatalysts for FOR and beyond.