The rheological properties of a dispersion of cellulose nanocrystals (CNCs) in an aqueous solution of polyoxyethylene (PEO) have been investigated. A peculiar behavior is reported. Upon adding CNC, the viscosity of the suspension first decreases and then increases. Adsorption of PEO chains on the surface of the nanoparticles has been suspected. Freeze-drying of this PEO-adsorbed CNC dispersion was performed, and the ensuing lyophilizate was extruded with low density polyethylene. Compared to neat CNC-based nanocomposites, both improved dispersibility and thermal stability were observed. This simple and physical method constitutes an approach of choice for the melt processing of CNC-based nanocomposites with a hydrophobic polymeric matrix applicable at the industrial scale.