The synthesis and functionalization of nitrogen-containing compounds continue to be important due to their wide applications. In particular, the preparation of nitriles and amides applying cost-effective and green methodologies is of central importance because these products represent valuable fine and bulk chemicals and serve as key precursors and central intermediates in organic synthesis and drug discovery as well as materials. Here, the preparation of nitriles and primary amides from alcohols and ammonia by a heterogeneous Cu-catalyzed aerobic oxidation process is reported. The optimal catalyst for this synthesis is based on supported copper oxide-nanoparticles, which are prepared by the impregnation and pyrolysis of simple copper nitrate on carbon. Applying these reusable nanoparticles, various simple, substituted, and functionalized aromatic, heterocyclic, and aliphatic nitriles are synthesized starting from inexpensive and easily accessible alcohols and ammonia in the presence of air. In addition, the synthesis of selected primary amides in a water medium is also performed using these Cu nanoparticles. © 2022 The Authors. Advanced Sustainable Systems published by Wiley-VCH GmbH.