Enzymes are the most efficient catalysts in nature that possess an impressive range of catalytic activities albeit limited by the stability in adverse condition. Functional peptides have emerged as alternative...

Spatiotemporal control for supramolecular polymerization has rendered a paradigm shift towards designing complex multi‐component supramolecular materials and derived nanocomposites. In this paper, we demonstrate self‐assembly/disassembly of amyloid‐inspired peptide nanostructures from Fmoc‐VFFAKK, 1 using gold nanoparticles (AuNPs)/cysteine mediated coupled equilibrium. We report the use of AuNPs to disaggregate the β‐sheets of the peptide nanofibers 1NF and twisted bundles 1TB to furnish dormant metastable nanoparticles. Upon cysteine mediated sequestration of the AuNPs the peptide fibers are regenerated. Such self‐assembly/disassembly of the fibers shows implication in tuning the mechanical strength of the resulting hydrogels. Further, a conformal coating of polydopamine (PDA) over the peptide fibers using the lysine amines furnishes rather robust fibers and orthogonally safeguard itself from AuNPs mediated disassembly of the fibers. Finally, such active coating with PDA having amine/quinone moieties allows selective attachment of AuNPs to furnish 1‐D organization of AuNPs over the coated peptide fibers.

Chiral polymers always have an edge over their achiral analogues owing to the effective utilization of the asymmetry to mimic nature in multiple ways. Chirality in tandem with conjugation in...