A method is provided for forming a substantially uniaxially-oriented, high content cellulose nanocrystal film. The method includes providing a plant-biomass-based suspension of cellulose nanocrystals and altering the pH of the cellulose nanocrystals to a substantially neutral pH. The suspension is sheared at a shearing rate. The method further includes orienting the cellulose nanocrystals in a substantially axial direction and removing water from the sheared cellulose nanocrystal suspension. As a result, a substantially uniaxially-oriented cellulose nanocrystal film is formed.