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Cellulose Nanocrystals The cover page illustrates cellulose nanocrystals extracted from trees, symbolizing nature's contribution to advanced materials. These nanocrystals align to form stratified thin films of varying thickness, each displaying vibrant, tunable colors. The artwork visually conveys the study's focus on environmentally friendly, optically active coatings, emphasizing the elegance and scalability of cellulose‐based materials for innovative applications. More details can be found in article 2400608 by Youssef Habibi and co‐workers.

Nature's most brilliant hues arise from the interaction of light with multilayered‐ structures of aligned building blocks. Mimicking this hierarchical organization in highly‐ordered thin films of liquid crystalline species has attracted increasing attention for potential applications in sensors and optical switching displays. Due to its intriguing ability to organize into optically active materials, cellulose nanocrystals (CNCs) are attracting a strong interest in the scientific community. This study demonstrates that the shear‐driven convective assembly technique can be used to stratify in a controlled fashion highly ordered multilayers of rod‐like CNC embedded in a protective hydrophobic polymer matrix leading to optically active thin films. The films remain fully transparent even after stratifying 50 layers. Atomic force microscopy analysis reveals that over 87% of the CNCs in the upper layer aligned within ±20° of the withdrawal direction. Notably, the stratification does not disrupt the organization of the underlying layers. The films exhibit strong selective reflections with uniform and intense colors, dependent on the number of stratified layers. This scalable appraoch enables precise control over the optical characteristics of CNC‐polymer composite films, presenting opportunities for environmentally friendly applications in pigment‐free coatings, security papers, and optical devices. Explore shear‐driven convective assembly's role in creating optically active thin films. Highly ordered multilayers of cellulose nanocrystals (CNCs) in a hydrophobic polymer matrix are achieved, offering precise control. The resulting films' optical activity, modulated by layer count, presents possibilities for pigment‐free coatings, security papers, and optical devices in this scalable, green technology.