A series of peptide-dendron conjugates, based on an intrinsically α-helical, alanine-rich sequence, were constructed to explore how the conformational equilibria of each structural element can be conformationally coupled. The interdendron spacing was varied from i, i+ 4 (2) to i, i+ 11 (9) to probe how the nature of the dendron interaction impacted the conformational properties. These studies revealed an α-helix to β-sheet conformational ...