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Tailorable chiral plasmonic nanostructures have attracted great interest due to their potential applications in photonics and sensing. However, there are limited straightforward fabrication routes to modulate the morphology of chiral materials with an external stimulus. Here, a helical assembly of gold nanospheres (AuNSs) is successfully obtained via self‐assembly using glycopeptide helical nanofibers as templates based on electrostatic interactions. The assembly morphology can be readily tailored from short debris to single‐/double‐ and multiple helical threads by changing pHs, resulting in well‐controlled modulation of circular dichroism (CD) in the visible range. Further, this tunable assembly and corresponding chiroptical properties are fully reversible in the pH range from 6 to 10. The electromagnetic simulation revealed how the structural geometries of AuNS helices changed the electromagnetic field propagation pattern to facilitate corresponding chiral optical properties. This approach is a unique and facilely obtained example of chiral nanomaterials with in situ tailoring morphology and chiral properties through external stimulus, demonstrating a potential application for biosensing. [ABSTRACT FROM AUTHOR]

Bacterial biofilms are troublesome in the treatment of bacterial infectious diseases due to their inherent resistance to antibiotic therapy. Exploration of alternative antibiofilm reagents provides opportunities to achieve highly effective treatments. Herein, we propose a strategy to employ self-assembled saccharide-functionalized amphiphilic metallacycles ( [2+2]-Gal , [3+3]-Gal , and [6+6]-Gal ) with multiple positive charges as a different type of antibacterial reagent, marrying saccharide functionalization that interact with bacteria via "sweet talking". These self-assembled glyco-metallacycles gave various nanostructures (nanoparticles, vesicles or micron-sized vesicles) with different biofilms inhibition effect on Staphylococcus aureus ( S. aureus ). Especially, the peculiar self-assembly mechanism, superior antibacterial effect and biofilms inhibition distinguished the [6+6]-Gal from other metallacycles. Meanwhile, in vivo S. aureus pneumonia animal model experiments suggested that [6+6]-Gal could relieve mice pneumonia aroused by S. aureus effectively. In addition, the control study of metallacycle [3+3]-EG 5 confirmed the significant role of galactoside both in the self-assembly process and the antibacterial efficacy. In view of the superior effect against bacteria, the saccharide-functionalized metallacycle could be a promising candidate as biofilms inhibitor or treatment agent for pneumonia.