In recent years, biomass-based adsorbents have attracted significant attention to remove Cr(VI) from aqueous solution due to their environmental friendliness, renewability, and biodegradability. In this work, TEMPO-oxidized cellulose nanofibrils (TOCNF) were prepared from bleached kraft pulp, and used as the matric. a novel biosorbent from cellulose nanofibrils bonded poly(m-aminobenzene sulfonate) was synthesized. Structural characterizations substantiated a successful grafting reaction between TOCNF and PABS. The biosorbent from TOCNF-PABS possessed a high nitrogen content of 7.0%. It exhibited excellent Cr(VI) adsorption capacity at the solution pH below 3, and almost 100% Cr(VI) can be removed. The adsorption of Cr(VI) on the biosorbent was described by a pseudo-second-order model and obeyed the Langmuir model. The Cr(VI) adsorption capacity of the biosorbent from TOCNF bonded PABS was almost ten times higher than that of TOCNF. 〈그림 본문 참조〉