Terahertz time-domain spectroscopy (THz-TDS) has expanded possibilities in cellulose crystallography research, as THz radiation detects most intermolecular vibrations and responds to the phonons of crystalline lattices. In this study, we traced the transformation of the cellulose crystalline lattice from cellulose I to cellulose II by THz-TDS and X-ray powder diffraction. Cellulose II was obtained by treating cellulose I with NaOH of different concentrations (0 wt%–20 wt%, at 2 wt% intervals). The THz absorption coefficient spectra of cellulose II showed three characteristic peaks (at 1.32 THz, 1.76 THz, and 2.77 THz). The THz absorption coefficient spectra of cellulose II treated with 20-wt% NaOH and cellulose I without NaOH treatment were fitted by a seventh-order Fourier series. Thus, the THz absorption coefficient spectra of samples treated with NaOH of other concentrations could be considered a combination of these two fitted profiles of cellulose I and cellulose II, multiplied by different coefficients. Furthermore, the coefficients could reflect the relative contents of cellulose I and cellulose II in the samples.