A series of Au Pd@C nanoalloy catalysts with tunable compositions were successfully prepared by a co-reduction method. The use of borane-tert-butylamine complex as reductant and oleylamine as both solvent and reductant was very effective for the preparation of the monodispersed nanoalloy. We evaluated the catalytic activity of these Au Pd@C nanoalloys for oxidative dehydrogenative coupling of aniline, which showed better catalytic activity than equal amounts of sole Au@C or Pd@C catalyst. The Au1Pd3@C catalyst exhibited the best performance, indicating that the conversion and selectivity were improved along with the increase of Pd composition. However, if the Pd composition was too high in the Au Pd alloy, Au1Pd7@C achieved only 81% conversion in this reaction. A series of Au Pd @ C nanoalloy catalysts with tunable compositions were successfully prepared by a co-reduction method. The use of borane-tert-butylamine complex as reductant and oleylamine as both solvent and reductant was very effective for the preparation of the monodispersed nanoalloy . The catalytic activity of these Au Pd @ C nanoalloys for oxidative dehydrogenative coupling of aniline, which showed better catalytic activity than equal amounts of the sole Au @ C or Pd @ C catalyst. The Au @ Pd3 @ C ​​catalyst showed the best performance, indicating that the conversion and selectivity were improved along with the increase of Pd composition. However, if the Pd composition was too high in the Au Pd alloy, Au1Pd7 @ C achieved only 81% conversion in this reaction.