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[Display omitted] • The Pt/Bi 2 O 3 interfaces undergo structural reconstruction during CV process and form highly dispersed Bi0 species on the surface of Pt aerogel. • Higher MOR activity in alkaline media was obtained for Bi0 decorated Pt aerogel. • The reaction kinetics is investigated by In-suit FTIR measurement and DFT calculations. Improving the activity and stability of electrocatalysts for methanol oxidation reaction (MOR) is key important for the large-scale application of direct methanol fuel cells (DMFCs). Herein, we provide a novel scheme to firstly build Bi-decorated Pt aerogel through the structural reconstruction of Pt/Bi 2 O 3 interface, which demonstrates an excellent mass activity of 7.99 A mg-1 Pt in MOR (8-fold higher than that of commercial Pt/C). Experimental results show that the synergistic effect between Bi0 species and Pt aerogel is the major cause of the improvement of the catalytic activity. In-suit Fourier transform infrared (FTIR) Spectroscopy results indicated that the generation and transformation of HCOO– intermediate are accelerated. Density functional theory (DFT) calculations indicate that the decorated Bi enhances the adsorption of OH species on the adjacent Pt site, which can facilitate the dehydrogenation of methanol and the removal of poisonous CO species. Thus, the electro-catalytic performance can be improved. This strategy can be extended to construct other types of interfaces, which may open new routes for the synthesis of highly efficient electrocatalysts. [ABSTRACT FROM AUTHOR]