A superhelix is a three-dimensional arrangement of a helix in which the helix is coiled around a common axis. Here, we are reporting a short 12-helix of α,γ-hybrid peptides terminated by metal binding ligands, self-assembled into a right-handed superhelix around a common axis in the presence of Cd(II) ions. Furthermore, these superhelices are assembled into hierarchical superhelical β-sheet-type structural motifs in single crystals. The results reported here may give new insights to construct advanced self-assembled architectures from peptide foldamers.