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N‐heterocyclic carbenes (NHCs) have garnered much attention due to their unique properties, such as strong σ‐donating and π‐accepting abilities, as well as their transition‐metal‐like reactivity toward small molecules. In 2015, we discovered that NHCs can react with nitric oxide (NO) gas to form radical adducts that resemble transition metal nitrosyl complexes. To elucidate the analogy between NHC...