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From a circular economyperspective, one-pot strategies for theisolation of cellulose nanomaterials at a high yield and with multifunctionalproperties are attractive. Here, the effects of lignin content (bleachedvs unbleached softwood kraft pulp) and sulfuric acid concentrationon the properties of crystalline lignocellulose isolates and theirfilms are explored. Hydrolysis at 58 wt % sulfuric acid resulted inboth cellulose nanocrystals (CNCs) and microcrystalline celluloseat a relatively high yield (>55%), whereas hydrolysis at 64 wt% gaveCNCs at a lower yield (