The cellulose nanocrystals(CNC) of uniform size are prepared by the high-pressure homogenization coupled with the sulfuric acid hydrolysis pretreatments in this paper. The CNC suspension is self-assembled to form a unique chiral arrangement with the ultrasonic treatment. The self-assembled CNC film is shaped further to possess novel structural color characteristics. The size and the morphology of the prepared CNCs are determined by the transmission electron microscope(TEM) and the scanning electron microscope(SEM). The CNCs are rod-like mostly and fully separated in suspension with highly uniform size, and possess the structural basis to form the chiral arrangement. From the surface potential, the sticky flow characteristics and the polarization characteristics, it is shown that at a higher sulfuric acid concentration, the zeta potential value and the viscosity of the CNC suspension are increased, which makes it easier to form the chiral arrangement. Further studies conclusively show that the CNCs are liable to self-assemble into the chiral arrangement after the ultrasonic treatment to exhibit excellent structural color characteristics.

cellulose nanofibers  /  chiral arrangement  /  structural color  /  rheology property  /  polarizing characteristic