LAUSR

Single‐atom catalysts have been demonstrated promising potential in diverse catalytic reactions; however, their practical application remains hindered by significant limitations in both activity and stability. Therefore, addressing how to effectively enhance their performance remains a critical challenge in the field of single‐atom catalysis. Herein, a Co single‐atom catalyst synergized with Co nanoparticles on a carbon support for oxidative coupling of benzyl alcohol and aniline into N‐benzylideneaniline in an O2 atmosphere is developed. The catalyst exhibits 95% conversion and 95% selectivity, a remarkable reaction rate enhancement (4 fold increase compared to an individual Co single‐atom catalyst), remarkable stability, and excellent substrate versatility. Furthermore, systematic investigations reveal that Co nanoparticles not only facilitate electron transfer between Co single‐atom sites and O2 but also serve as an enrichment site for aniline molecules, thereby preventing strong adsorption of aniline onto Co single‐atom sites. These findings provide new insights into the rational design of high‐performance single‐atom catalysts for multi‐step organic transformation through combining with bifunctional nanoparticles.