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N‐Brominated compounds are widely used in synthetic and industrial chemistry. In addition, N‐brominated species are implicated in the development of numerous inflammatoryrelated diseases. In this study by Robert J. O'Reilly and Amir Karton (DOI: 10.1002/qua.25024), accurate NBr bond dissociation energies for a diverse set of molecules have been obtained by means of the high‐level W2 composite protocol. This article focuses on the effect of structure on the strength of NBr bonds toward the formation of free radicals. Additionally, to facilitate the study of other N‐brominated species, a large number of more economical theoretical procedures have been assessed for the computation of accurate NBr bond energies.