Nanocrystalline cellulose (NCC) has shown great potential for reinforcing nanocomposite systems, particularly in biopolymer-based nanocomposites. In the present work, transparent and biodegradable chitosan (CH)/guar gum (GG)/NCC nanocomposite films were designed and prepared. The effect of NCC loadings on the rheological behavior of the as-prepared nanocomposite suspensions was investigated, the overall properties of the resultant nanocomposite films as a function of various amounts of NCC were determined, and the surface morphology of various nanocomposite films was characterized by scanning electron microscopy (SEM). Results indicated that the increased NCC loadings increased the shear viscosity of the nanocomposite suspensions. Moreover, as expected, the obtained CH/GG/NCC nanocomposite films were found to exhibit improved tensile strength and reduced air permeability in comparison to pure CH/GG films. This work supported the conclusion that NCC was effective in reinforcing the CH/GG composite films, which may be a promising material for food packaging applications.