Crystallinity is an essential indicator for evaluating the quality of fiber materials. Terahertz spectroscopy technology has excellent penetrability, no harmful substances, and commendable detection capability of absorption characteristics. The terahertz spectroscopy technology has great application potential in the field of fiber material research, especially for the characterization of the crystallinity of cellulose. In this work, the absorption peak of wood cellulose, microcrystalline cellulose, wood nano cellulose, and cotton nano cellulose were probed in the terahertz band to calculate the crystallinity, and the result compared with XRD and FT-IR analysis. The vibration model of cellulose molecular motion was obtained by density functional theory. The results showed that the average length of wood cellulose (WC) single fiber was 300 μm. The microcrystalline cellulose (MCC) was bar-like, and the average length was 20 μm. The cotton cellulose nanofiber (C-CNF) was a single fibrous substance with a length of 50 μm, while the wood cellulose nanofiber (W-CNF) was with a length of 250 μm. The crystallinity of cellulose samples in THz was calculated as follows: 73% for WC, 78% for MCC, 85% for W-CNF, and 90% for C-CNF. The crystallinity values were obtained by the three methods which were different to some extent. The absorption peak of the terahertz spectra was most obvious when the samples thickness was 1 mm and mixed mass ratio of the polyethylene and cellulose was 1:1. The degree of crystallinity was proportional to the terahertz absorption coefficients of cellulose, the five-movement models of cellulose molecules corresponded to the five absorption peak positions of cellulose.