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Herein, we demonstrate that C18\u2010epimerization of glycyrrhizic acid (GA) acts as a molecular switch to modulate both its self\u2010assembly behavior and the properties of the resulting supramolecular hydrogels. Computational simulations and experimental analyses reveal that this epimer transition induces a \u201cdomino effect\u201d that fundamentally rewrites the self\u2010assembly pathway, particularly by reshaping the intermolecular hydrogen\u2010bonding (H\u2010bond) network. Isoglycyrrhizic acid (IGA), the C18\u2010epimer of GA, forms a densely crosslinked fiber network through a distinct tetramer stacking mode, with significantly enhanced H\u2010bond interactions arising from altered electrostatic surface potential and molecular planarity. These structural differences yield hydrogels with enhanced injectability and viscosity, supporting the translational potential of IGA\u2010based hydrogel platforms. 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