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The α,β‐unsaturated γ‐lactams have been found in many biologically active peptide natural products. Due to their biological activities, extensive efforts have been made in the literature to synthesize the α,β‐unsaturated γ‐lactams. Here, we are reporting the spontaneous transformation of E‐α,β‐unsaturated γ‐amino acids into α,β‐unsaturated γ‐lactam through in‐situ activation of free carboxylic acid...