Hierarchical superhelical architectures and dynamic chirality inversion are central to nature's adaptability and functionality, yet replicating these features in synthetic systems remains a significant challenge. Previously, we developed a chemical reaction network for the creation of programmable transient supramolecular chiral G-quadruplex hydrogels.1 Later, we demonstrate the use of chemical fuels for regulating self-assembly pathway, which thereby controls the supramolecular chirality of assembly in non-equilibrium systems.2 Herein, we present a supramolecular gel system that achieves autonomous gel-to-gel transformations and reversible chirality inversion between superhelix and single-helix configurations, all without passing through a sol phase.3 This behavior fundamentally differs from traditional gel-sol-gel systems, which require disassembly to achieve chirality inversion. This system mimics collagen-like hierarchical organization and dynamic chirality adaptation, bridges the gap between static hierarchical assemblies and truly dynamic systems, paving the way for the design of functional soft matter with biomimetic adaptability.

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