AbstractCotton linter pulp was oxidized in the TEMPO-NaBr-NaClO system with ultrasonic treatment, and cellulose nanocrystals having high carboxylate content were produced directly. Results showed that the C6 primary hydroxyl group of cellulose fiber was converted to the carboxylate group, whose amount could be up to 1.66 mmol/g. During the oxidizing reaction, some of the amorphous region in the cellulose fiber was modified and gradually hydrolyzed, but the crystalline region still remained. It was also shown by TEM (Transmission electron microscopy) that the widths of cellulose nanocrystals were approximately 5-10 nm, and the lengths were approximately 100-400 nm. The high carboxylate content cellulose nanocrystals could be produced in one step by this method, yielding a stable and well dispersed aqueous suspension.