Polyurethane (PU) nanocomposites utilizing cellulose nanocrystals (CNCs) as nanofiller and amorphous PU matrix were synthesized in a novel solvent-free bulk process. A green nanofiller, CNCs, was studied as reinforcement and was further modified by grafting poly(ethylene glycol) (PEG) on the CNC surface (CNC-PEG). Transmission electron microscopy revealed an excellent dispersion of the PEGylated CNC nanoparticles in the PU matrix, whereas as-received CNCs formed agglomerates. The results indicated strong improvements in tensile properties with Young's modulus increasing up to 50% and strength up to 25% for both, PU/CNC and PU/CNC-PEG nanocomposites. The enhanced tensile modulus was attributed to stiff particle reinforcement together with an increase in glass transition temperature.