The rheological behavior of aqueous suspensions of lignocellulose nanofibrils (LCNFs) is investigated systematically by considering the coupled effect of residual lignin and LCNF morphology. The LCNF was obtained by high-energy fluidization of TEMPO-oxidized mechanical fibers, followed by size fractionation (fibril widths of ∼5, ∼9, and ∼18 nm). The nanofibril width and the corresponding fibril-fibril interactions are strongly influenced by the presence and distribution of lignin in the respective fractions, either retained on the fibril surface or as free structures present in the finest size fraction. All samples containing lignin display dilatancy, typifying gel suspensions with aggregated hydrophobic particles. Fine fractionated samples display strong gel behavior. The coarse fractionated sample, by contrast, shows a greater tendency to flocculate via entanglement and displays less gel-like characteristics; hence, it dewaters more freely.