Twin-screw extrusion (TSE) is a rather recent method to produce cellulose nanofibrils (CNFs) at a high solid content under continuous feeding. Here, never-dried commercial eucalyptus pulp was used as starting material to produce CNFs by TSE after a chemical pretreatment to introduce carboxylic groups via TEMPO-mediated oxidation and carboxymethylation. Five samples with acarboxyl content ranging from 800 to 1300 µmol.g-1 were produced to explore how the carboxyl content affects the aptitude of cellulose fibers to be broken down to nanoscale. The properties of the resulting CNFs in terms of nanosized fraction, morphology and rheological properties were investigated. A critical carboxyl content of 700 µmol.g-1was a prerequisite for the successful conversion of cellulose fibers into a CNF gel by TSE, regardless the pretreatment method. The degree of swelling of the fibers was put forward to account for this critical parameter.

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