The Aromatic Cope Rearrangement is a highly challenging chemical reaction under thermal conditions, primarily attributed to the loss of aromaticity during the initial [3,3] sigmatropic step of the process. This scarce transformation requires typically high temperatures and engineered 1,5-hexadiene scaffolds, where one double bond is included in an aromatic ring, making it impractical for a straightforward synthesis of new molecules. Employing gold(I) catalysts, the energetic barriers associate to this rearrangement can be drastically decreased allowing to perform, in mild conditions and high yields, the diastereoselective and divergent aromatic Cope rearrangement or the selective dearomatization reaction from various α-allyl-α’-heteroaromatic γ-lactone or malonate derivatives. These data are the primary NMR FID files of all new compounds of this study.