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 un...