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Industrial production of low-charge microfibrillated cellulose (MFC) typically results in wide fibril size distributions. This polydispersity influences viscosity, overall colloidal stability, and rheological properties of MFC suspensions and gels in aqueous systems. In this work, a systematic rheological analysis is performed for industrially prepared MFC and fractions of different size distributions. Gel formation and flow characteristics (e.g., shear-thinning) of each fraction are examined under neutral and acidic conditions and compared with the unfractionated MFC suspension. The effects of size, aspect ratio, and surface charge on the rheology of semi-dilute MFC suspensions are discussed. The results demonstrate that particle size and aspect ratio distribution control the viscoelasticity and shear-thinning properties of MFC suspensions. An increased fraction of small diameter nanofibrils, by ex situ addition of the fine particles with high aspect ratio or removal of the coarsest particles (with lower aspect ratio) by fractionation, significantly enhances the storage modulus and the yield stress of the complex mixture, compared to the properties of the coarser fractions. New insights are also reported on the tailoring of the rheology of highly polydisperse fibrillar mixtures, where the rheological contributions of each fraction are discussed. Graphic abstract

The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.202204800.