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However, the structural polymorphism of the bioinspired self\u2010assemblies poses challenges for their rational design and scale production as sustainable, eco\u2010friendly, and tailorable materials for technology applications. Here, it is demonstrated that peptide polymorphic crystallization is a hierarchical process, evolving from initially flexible, twisted nanofibrils bundling to form ribbons, then ripening to robust, plate\u2010like crystals composed of superhelices, as observed using high\u2010resolution microscopy and crystallography supported by molecular dynamics simulations and quantum mechanical calculations. The hierarchical process accounts for the known morphological diversity of peptide crystals and provides a mechanism of controllably restricting the assembly to create only specific supramolecular structures as demanded. Especially, the superhelical organization enables high\u2010efficiency energy transformation, resulting in tremendous photoluminescent, optical waveguiding, and electromechanical energy\u2010harvesting potential. 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