Cellulose-based nanocomposites are promising materials to replace the fossil-based polymers since they are biodegradable and produced from renewable resources. However, achieving good dispersion of nanocellulose in the matrix is one of the main obstacles because nanomaterials tend to form aggregates and lose their merits. In this study we developed an in-situ polymerization method to produce cellulose nanocrystals reinforced polyvinyl acetate, and the method of direct mechanical mixing was used as reference. The stability of in-situ and mixed nanocomposite aqueous dispersions was investigated by zeta potential measurements, and the results show that both of them were electrostatic stable at pH 4. Atomic force microscopy (AFM) and scanning electron microscopy (SEM) were used to characterize the dispersion of cellulose nanocrystals in the in-situ and mixed nanocomposites after drying, and better dispersion could be seen in the in-situ samples compared with the mixed ones. Tensile testing showed that the in-situ nanocomposites with same cellulose content had higher strength and longer elongation at break compared to the mixed nanocomposites. Furthermore, crosslinking the cellulose and partially hydrolyzed polyvinyl acetate with sodium tetraborate was also performed to further improved the reinforcing efficiency. The results from Raman spectroscopy illustrate that the heavy atoms (CC and CO) in cellulose experienced more stretching in the crosslinked nanocomposites, and the tensile testing indicated the elastic modulus and ultimate strength of them were increased significantly than those without crosslinking.