We report a series of coordination cages that incorporate peptide chains at their vertices, prepared through subcomponent self‐assembly. Three distinct heterochiral tripeptide subcomponents were incorporated, each exhibiting an L−D−L stereoconfiguration. Through this approach, we prepared and characterized three tetrahedral metal‐peptide cages that incorporate thiol and methylthio groups. The gelation of these cages was probed through the binding of additional metal ions, with the metal‐peptide cages acting as junctions, owing to the presence of sulfur atoms on the peripheral peptides. Gels were obtained with cages bearing cysteine at the C‐terminus. Our strategy for developing functional metal‐coordinated supramolecular gels with a modular design may result in the development of materials useful for chemical separations or drug delivery.