The coordination chemistry of short chain peptides with transition metals is described in terms of the available crystal structures. Despite their high interest as synthetic models for metalloproteins and as building blocks for molecular materials based on the tuneable properties of oligopeptides, single crystal X-ray diffraction studies are scarce. A perusal of the most relevant results in this field allows us to define the main characteristics of oligopeptide–metal interactions, the fundamental problems for the crystallization of these complexes, and some hints to identify future promising approaches to advance the development of metallopeptide chemistry.