Abstract A green and general method for the direct transformation of aldehydes to nitriles was developed. This method features a broad scope of substrates including aromatic, heterocyclic, and aliphatic aldehydes, by using I 2 /NH 4 Br in aqueous ammonia. Readily available aldehydes can be smoothly converted to corresponding nitriles in one‐step under open air at room temperature for 1–12 hours. This protocol is transition‐metal‐free and could be applied for the synthesis of various key cyano (CN)‐containing molecules.