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Engineering free-standing 2D nanomaterials with compositional, spatial, and functional control across size regimes from the nanoto mesoscale represents a significant challenge. Herein, we demonstrate a straightforward strategy for the thermodynamically controlled fabrication of multicomponent sectored nanosheets in which each sector can be chemically and spatially addressed independently and orthogonally. Collagen triple helices, comprising collagen-mimetic peptides (CMPs), are employed as molecularly programmable crystallizable units. Modulating their thermodynamic stability affords the controlled synthesis of 2D core−shell nanostructures via thermally driven heteroepitaxial growth. Structural information, gathered from SAXS and cryo-TEM, reveals that the distinct peptide domains maintain their intrinsic lattice structure and illuminates various mechanisms employed by CMP triple helices to alleviate the elastic strain associated with the interfacial lattice mismatch. Finally, we demonstrate that different sectors of the sheet surface can be selectively functionalized using bioorthogonal conjugation chemistry. Altogether, we establish a robust platform for constructing multifunctional 2D nanoarchitectures in which one can systematically program their compositional, spatial, and functional properties, which is a significant step toward their deployment into functional nanoscale devices.

Seeded Heteroepitaxial Growth of Crystallizable Collagen Triple Helices: Engineering Multifunctional Two-Dimensional Core Shell Nanostructures