Chemical shift tensor of cellulose Iα was investigated via line-shape simulations of solid-state 13 C NMR spectra obtained for uniaxially oriented cellulose nanocrystals (CNCs). The cellulose film composed of highly oriented CNCs was obtained by shearing of a CNC/water suspension. The solid-state 13C NMR measurements were performed at different angles (βLs), which are defined as angles between the static magnetic field and the direction of uniaxial orientation of CNC. The shape of the obtained NMR spectra varied depending on the βL. The line-shape simulations for the series of the solid-state 13C NMR spectra indicate that the directions of δ33 axis of C2-C6 locate almost parallel to the directions of C-O bonds.
