Optically Controlled Peptide-Based Reconfigurable Folding via Regular Monodisperse Azobenzene Arrangement.

Reconfigurable nanostructures featuring geometric deformation present a viable alternative to the canonical disintegration-reassembly paradigm in nanotechnology, however, their implementation in peptide-based supramolecular nanosystems remains challenging. This difficulty stems from a fundamental conflict between structural integrity and reconfigurability─a conflict rooted in the inadequate orthogonality between the framework bonds and reconfigurable bonds. Here, we utilized robust homotetrameric peptide coiled-coils to arrange azobenzene molecules monodispersely and regularly in a two-dimensional (2D) single-molecular plane, creating a new architecture of peptide supramolecular system, called monolayered peptide-AZO nanosheets (MPANs). This design not only effectively decouples the nanostructure's framework bonds from the reconfigurable bonds of azobenzene but also ensures the parallel alignment of monodisperse azobenzene units. Consequently, azobenzene-incorporated MPANs undergo photoinduced reversible multilayer folding into three-dimensional (3D) nanostructures. Remarkably, MPANs demonstrate tailorable surface chemistries that dictate folding morphology, yielding accordion-like, carambola-shaped, and rosette pillar-shaped 3D nanostructures. This work resolves bond orthogonality issues in peptide-based supramolecular reconfiguration through the isolation and dispersion of reconfigurable bonds, and also provides a versatile strategy for constructing morphologically controllable nanostructures, thereby aiding the development of advanced peptide nanodevices.