A water-based polyurethane (PUR) acrylate water emulsion was selected as a radiation curable matrix for preparing nanocomposites including cellulose nanocrystals (CNC) prepared by controlled hydrolysis of Ramie fibers. Cross-linking polymerization of samples prepared in the form of films or of 1 mm-thick bars was either initiated by exposure to the 395 nm light of a high intensity LED lamp or by treatment with low energy electron beam (EB). The conversion level of acrylate functions in samples submitted to increasing radiation doses was monitored by Fourier Transform Infrared Spectroscopy (FTIR). Differential Scanning Calorimetry (DSC) and Dynamic Mechanical Analysis (DMA) were used to characterize changes in the glass transition temperature of the PUR-CNC nanocomposites as a function of acrylate conversion and of CNC content. Micromechanical testing indicates the positive effect of 1 wt% CNC on Young’s modulus and on the tensile strength at break (σ) of cured nanocomposites. The presence of CNC in the PUR acrylate matrix was shown to double the σ value of the nanocomposite cured to an acrylate conversion level of 85% by treatment with a 25 kGy dose under EB, whereas no increase of σ was observed in UV-cured samples exhibiting the same acrylate conversion level. The occurrence of grafting reactions inducing covalent linkages between the polysaccharide nanofiller and the PUR acrylate matrix during the EB treatment is advanced as an explanation to account for the improvement observed in samples cured under ionizing radiation.