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Although it is well known that the amazing iridescent colors of the cuticle of beetles reflect the intricate nanoscale organization of bio‐fibers, artificial inorganic materials with comparable optical responses have not yet been synthesized from abiotic nanoscale building blocks. Such materials could find broad applications, including in circular polarizers, to generate circularly polarized luminescence, or in lasers. Herein, we describe a general method for the fabrication of biomimetic chiral photonic crystals by Langmuir–Schaefer assembly of colloidal inorganic nanowires. We not only reproduced the intricate helical structure and circularly polarized color reflection observed in beetles, but also achieved the highest chiroptical activity with a dissymmetry factor of −1.6 ever reported for chiral inorganic nanostructures. More importantly, the programmable structural control based on the precise interlayer arrangement endows us with unprecedented freedom to manipulate the optical activity of as‐fabricated chiral photonic crystals. [ABSTRACT FROM AUTHOR]

An ultrastrong and broadband chiroptical response is key but remains challenging for many device applications. A simple and cost-effective bottom-up method is introduced to fabricate large-area long-range ordered chiral ultrathin films with the Langmuir-Schaeffer technique using gold nanowires as building blocks. Significantly, as-prepared ultrathin films display giant optical activity across a broad wavelength range covering visible and near infrared regions with an anisotropic factor of up to 0.285, which is the record value for bottom-up techniques. Detailed experimental result and theoretical analysis disclose that such remarkable optical activity originates from birefringence and dichroism of the well-aligned Au nanowire layers in the ultrathin films. The universality of this facile strategy for constructing chiral ultrathin films is further demonstrated with many other one-dimensional nanomaterials. [ABSTRACT FROM AUTHOR]