Alternating Stacking of Nanocrystals and Nanofibers into Ultrastrong Chiral Biocomposite Laminates

Attaining high mechanical strength and flexibility for chiral nematic biopolymer composites without compromising their vivid optical iridescence is an intriguing but challenging task. Traditional cellulose nanocrystal (CNC) blend nanocomposite films typically lose their coloration and display weak mechanical performance due to poor load transfer between needle-like nanocrystals and the collapse of a twisted organization. Herein, we report a design of robust laminated biocomposites with an alternatively stacked chiral nematic CNC phase and a random cellulose nanofiber (CNF) phase via a hydrogen-bonding-assisted layer-by-layer method. In contrast to the traditional biopolymer blends, the alternating CNC-CNF stacked films possess many-fold enhancement in both mechanical strength and toughness with their vivid structural colors highly preserved. We suggest that the enriched hydrogen bonding and partial limited entanglements at the interfaces between the helicoidal and random phases are responsible for enhancing the mechanical performance of robust biocomposites with brilliant iridescent colors. Such organized cellulose-cellulose biocomposites with alternating helicoidal-random phases fabricated by a facile sequential strategy may facilitate the development of sustainably sourced, damage-tolerant, and photonic films for bioenabled display technologies, security indicators, soft robotics, camouflages, and pressure sensors.