Construction of strong, tough, and stiff biophotonic materials with customized and extended optical performance is significant to expand sustainable optics while it remains challenging. Herein, we propose a vacuum-assisted layer-by-layer assembly of cellulose nanocrystal and cellulose nanofiber alternatingly to fabricate nanocellulose photonic laminates. This strategy leverages the VASA technique to regulate drying kinetics and the layer-by-layer method to harmlessly incorporate energy-dissipating phases, enabling the fabrication of homogeneous and densely-packed nanocellulose photonic laminates with finely- tailored optomechanical performances. Specifically, the resultant nanocellulose photonic laminates synergistically integrate load-bearing cellulose nanocrystal sublayers and energy-dissipating cellulose nanofiber sublayers, achieving a comprehensive combination of high strength, toughness, stiffness, and impact resistance. Moreover, the resulting nanocellulose photonic laminates demonstrate well controllability and flexible editability in stacking structure via layer-by-layer assembly variation, that enables versatile optical functionalities, including arbitrary color blending based on the RGB color model and machine-learning-assisted color prediction. Impressively, by integrating nanocellulose photonic laminates with diverse stacked architectures, we establish a photonic matrix platform featuring programmable color-switching responses for information encoding and encryption. This work takes a crucial step forward to sustainable photonic materials with excellent mechanical combinations and optical functionality for bio-enabled display technologies and security indicators.

Color-changeable smart textiles capable of converting external stimulus into change in eye-perceptible colors are promising for visual sensor and wearable devices. However, conventional color-changeable smart textiles based on functional chemical dyes suffer the narrow-ranged color shifting and hence the bad visual interaction resolution. In this work, inspired by that chameleon rapidly tuning skin iridescence through active tuning of guanine nanocrystal spacing, a full-color-changeable textile equipped with a cholesteric photonic skin is developed via layer-by-layer assembly strategy by using sustainable nanocellulose as photonic ink to work with graphene oxide as light absorber and polyvinyl alcohol as plasticizer. After assembled, a multi-phase layered stacking coupled with Janus surface structure forms, hence generating structural synergic effects bringing multi functions for the resulting photonic textile, including flexible optical adjustability, strong-tough combination, hydration-setting formability, and progressive wettability. More impressively, resultant photonic textiles present wide-ranged color-shifting capability with a high identifiability outperforming most of conventional color-changeable textiles, demonstrating great feasibility to monitor the directional water transport process, diverse organic componence volatilization, and ambient humidity, in a naked-eye-readable, real-time, and quantifiable manner.