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Abstract We demonstrate shear‐printed layered photonic films with vivid structural coloration from bio‐derived cellulose nanocrystals and highly aligned Ti₃C₂T_xMXene nanoflakes. These ultrathin films (700–1500 nm) show high light transmittance above 40% in the visible range. In reflectance mode, however, the films appear vividly colored and iridescent due to the multiple distinct photonic bandgaps in the visible and near‐infrared ranges, which are rarely observed in CNC composites. The structural coloration is controlled by the stacking of MXene nanoscale‐thin layers separated by the thicker cellulose nanocrystals matrix, as confirmed by photonic simulations. The unique combination of distinctly different optical appearances in transmittance and reflectance modes occurs in films printed with just a few layers. This is because of the molecularly smooth interfaces and the high refractive contrast between bio‐based and inorganic phases, which result in a concurrence of constructive and destructive interference. These lamellar biophotonic films open the possibilities for advanced radiative cooling, camouflaging, multifunctional capacitors, and optical filtration applications, while the cellulose nanocrystals matrix strengthens their flexibility, robustness, and facilitates sustainability. 

Stacking atomically thin two-dimensional (2D) nanosheet materials leads to unique synergy in their inherent properties due to an intimate combination and matching that is not possible via separate individual components and phases. However, traditional synthesis and assembly methods result in poor architectural control and restricted surface chemistry, thereby limiting their prospective potentials. This brief overview provides consideration of different synthesis and assembly methods for fabrication of diverse novel heterostructures. The advantages and challenges of existing methods are discussed. Finally, future perspectives regarding crafting of heterostructures with highly controllable architectures and interfacial/surface chemistry, and advanced characterization methods are highlighted. 

Abstract The integration of chiral organization with photonic structures found in many living creatures enables unique chiral photonic structures with a combination of selective light reflection, light propagation, and circular dichroism. Inspired by these natural integrated nanostructures, hierarchical chiroptical systems that combine imprinted surface optical structures with the natural chiral organization of cellulose nanocrystals are fabricated. Different periodic photonic surface structures with rich diffraction phenomena, including various optical gratings and microlenses, are replicated into nanocellulose film surfaces over large areas. The resulting films with embedded optical elements exhibit vivid, controllable structural coloration combined with highly asymmetric broadband circular dichroism and a microfocusing capability not typically found in traditional photonic bioderived materials without compromising their mechanical strength. The strategy of imprinting surface optical structures onto chiral biomaterials facilitates a range of prospective photonic applications, including stereoscopic displays, polarization encoding, chiral polarizers, and colorimetric chiral biosensing.