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However, due to their strong aggregating tendency, the precise control of the self\u2010assembly of \u03b2\u2010sheet\u2010forming peptides remains a challenge. We propose a molecular geometry strategy to study and control the self\u2010assembly of cross\u2010\u03b2 structures. We conjugate the peptide with shape\u2010persistent polyhedral oligomeric silsesquioxane (POSS), which acts as a hydrophilic head and senses the solvent environment. The POSS\u2010peptide amphiphiles display two distinct self\u2010assembly pathways: twisted nanoribbons transforming into either nanotubes at low water content or flat nanoribbons at high water content. The peptide packing in flat nanoribbons is predominantly modulated by POSS, diverting the system away from crystal formation, which is the absolute lowest energy state of pure peptide self\u2010assemblies. For the first time, we have demonstrated that POSS can serve as a useful tool to adjust the interactions between cross\u2010\u03b2 strands, achieving fine\u2010tuning of the pathway complexity (i.e., the kinetic and thermodynamic aspects of peptide self\u2010assembly). With this versatile molecular platform incorporating multiple functionalities of POSS and programable peptide sequences, this study provides a platform to exploit cross\u2010\u03b2\u2010based nanomaterials with functional and pathological significance.<\/jats:p>","DOI":"10.1002\/anie.202420043","type":"journal-article","created":{"date-parts":[[2024,12,23]],"date-time":"2024-12-23T22:55:43Z","timestamp":1734994543000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Engineering the Self\u2010Assembly Pathways of POSS\u2010Peptide Amphiphiles to Form Diverse Cross\u2010\u03b2 Structures"],"prefix":"10.1002","volume":"64","author":[{"given":"Zhen","family":"Du","sequence":"first","affiliation":[{"name":"South China Advanced Institute for Soft Matter Science and Technology School of Emergent Soft Matter South China University of Technology  Guangzhou 510640 China"},{"name":"Guangdong Provincial Key Laboratory of 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