Hydrogels are three-dimensional networks of hydro-soluble polymers containing a large amount of water that have found a wide panel of applications in many sectors. The need for eco-friendly and nontoxic materials for the elaboration of sustainable hydrogels is obvious, and materials derived from biomass can easily meet these requirements. Cellulose nanocrystals (CNC) and arabinoxylans (AX) are abundant, biobased, hydrophilic, and renewable nanoparticles and polymers that interact together. In this study, we have built fully biobased hydrogels using CNC and AX. First, as revealed by Quartz Crystal Microbalance with Dissipation (QCM-D) experiments, AX adsorbs almost instantly on cellulosic surfaces in an irreversible manner. Nevertheless, gelation kinetics is not instantaneous and shows temperature dependence. The determination of phase diagrams using the inverted tube method leads to the conclusion that high AX/CNC ratios are needed for gel formation. The mechanical properties of CNC-AX hydrogels were investigated by measuring storage and loss moduli (G', G '') as a function of concentrations and hydrogel reformation after submission to high shear rates. Hydrogel properties were also tuned by increasing the ionic strength and the enzymatic removal of arabinose moieties from AX. In light of the obtained results, we hypothesize that gel formation occurs in two steps, i.e., AX adsorption followed by gelation of the complexes, and is due to the formation of reversible and tunable interactions between CNC/AX complexes interacting with each other, offering a wide panel of physicochemical tools to tune and trigger the final properties of hydrogels.