Among the greatest challenges in the field of microporous solids is the development of ''smart'' materials, displaying environment-triggered property tuning. These could be used both in traditional and new applications of microporous materials. In this context, supramolecular peptide-based solids have recently emerged as interesting alternatives to standard microporous solids, such as zeolites and carbon molecular sieves. They possess framework and conformational flexibility, are kinetically stable and reasonably thermally resistant. Important properties such as pore size and inner wall chemistry can be controlled through appropriate chemical modification of the peptide molecules. Peptide-based porous solids have permanent microporosity, often with molecularly sized cavities created by removal of co-crystallised solvent. Some have already been successfully tested as adsorbents and permselective materials, confirming their potential. This review covers the identification, synthesis, characterization techniques and properties of peptide-based microporous solids, discussing their most unique functionalities.