As a wise and profound teacher, nature provides numerous creatures with rich colors to us. To biomimic structural colors in nature as well as color changes responsive to environmental stimuli, there is a long way to go for the development of free-standing photonic films from natural polymers. Herein, a highly flexible, controllably iridescent, and multistimuli-responsive cellulose nanocrystal (CNC) film is prepared by simply introducing a small molecule as both plasticizer and hygroscopic agent. The presence of the additive does not block the self-assembly of CNC in aqueous solution but results in the enhancement of its mechanical toughness, making it possible to obtain free-standing iridescent CNC films with tunable structural colors. In response to environmental humidity and mechanical compression, such films can change structural colors smoothly by modulating their chiral nematic structures. Notably, the chromism is reversible by alternately changing relative humidity between 16 and 98%, mimicking the longhorn beetle Tmesisternus isabellae. This chromic effect enables various applications of the biofilms in colorimetric sensors, anticounterfeiting technology, and decorative coatings.
Keywords: cellulose nanocrystal; chiral nematic structure; environmental stimuli-responsive chromism; flexibility; structural color.