(Hetero)aromatic and aliphatic nitriles constitute major building blocks for organic synthesis and represent a versatile motif found in numerous medicinally and biologically important compounds. In general, these nitriles are synthesized by traditional cyanation procedures using toxic cyanides. With respect to green chemistry, the development of more sustainable and cost-efficient processes for the synthesis of advanced nitriles is highly desired. Here we report an environmentally benign synthesis of all kinds of structurally diverse aryl, heterocyclic, allylic and aliphatic nitriles from easily available alcohols applying aqueous ammonia and molecular oxygen. Key to success for this synthesis is the use of nitrogen-doped graphene-layered non-noble metal oxides as stable and durable nanocatalysts. As an example a renewable synthesis of adiponitrile, an industrially important bulk chemical is presented.