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[Display omitted] • Oxygen vacancies enhance the interaction between the support and Pd-Co NPs. • Co atom strengthens the adsorption of reactants on the Pd atoms. • Pd-Co/TiO 2 -Vo shows excellent small molecule reduction performance. Small molecules are converted into high-value products through electrochemical methods, which are considered as potential substitutes for traditional industrial methods. To reduce the use of precious metal and modulate the local environment by oxygen vacancies, Pd-Co nanoalloys supported on TiO 2 with oxygen vacancies (Vo) are prepared through a facile pyrolysis approach. The superior ORR performance is obtained comparing to the commercial Pt/C (20 wt%) catalysts in alkaline solution. Moreover, the catalyst has amazing catalytic activity for NRR. The synergistic effect of Pd-Co alloys and the Vo greatly improves the yield of NH 3 (4.11 µg/(h·cm2)) and the Faradaic efficiency (2.83%). The performance of small molecular reduction is enhanced by the strong metal-support interactions (SMSI), which agree with the density functional theory (DFT) calculations results. It is anticipated that the established nanoalloy electrocatalysts with modulation of metal–support interactions provide guidance for designing heterogeneous electrocatalysts with high efficiency. [ABSTRACT FROM AUTHOR]