Despite their concomitant emergence in the 1990s, γ‐peptide foldamers have not developed as fast as β‐peptide foldamers and to date, only a few γ‐oligomer structures have been reported, and with sparse applications. Among these examples, sequences containing α,β‐unsaturated γ‐amino acids have recently drawn attention since the Z/E configurations of the double bond provide opposite planar restrictions leading to divergent conformational behaviors, from helix to extended structures. In this Review, we give a comprehensive overview of the developments of γ‐peptide foldamers containing α,β‐unsaturated γ‐amino acids with examples of applications for health and catalysis, as well as materials science.