Microfibrillated cellulose isolated from bagasse was used to prepare novel nanocomposites using cross-linked gelatin as a biodegradable polymer matrix. Microfibrillated cellulose loadings up to 25% (weight percent) were used. The prepared nanocomposites were characterized regarding their wet and dry tensile strength, water sorption, and water vapor permeability. Nanocomposites’ surfaces were examined by scanning electron microscopy; the scanning electron microscopy images indicated homogeneous distribution of microfibrillated cellulose in the gelatin matrix. Microfibrillated cellulose improved wet and dry maximum tensile stress and modulus of cross-linked gelatin but resulted in a decrease of its strain at break. Microfibrillated cellulose did not affect the water absorption of cross-linked gelatin but significantly improved its moisture barrier property.