Herein, hybrid k-carrageenan bio-nanocomposite films were fabricated by using two types of nanofillers, organically modified montmorillonite (OMMT), and cellulose nanocrystals (CNCs). Hybrid bio-nanocomposite films were made by casting techniques employing 4 wt% of CNCs, OMMT, and hybridized CNCs/OMMT in a 1:1 ratio. The rheological and morphological properties and thermal stability of all composites were investigated using rotational rheometry, thermogravimetry analysis, differential scanning calorimetry, field emission scanning electron microscopy, and transmission electron microscopy (TEM). The results showed that the hybrid CNC/OMMT bio-nanocomposite exhibited significantly improved properties as compared to those for the bio-nanocomposites with single fillers due to the nanosize and homogenous nanofiller dispersion in the matrix. Rheological analysis of the hybrid bio-nanocomposite showed higher dynamic shear storage modulus and complex viscosity values when compared to those for the bio-nanocomposite with individual fillers. The TEM analysis of the hybridized CNC/OMMT bio-nanocomposite revealed that more particles were packed together in the CNC network, which restricted the matrix mobility. The heat resistance and thermal stability bio-nanocomposite k-carrageenan film enhanced rapidly with the addition of hybridized CNCs/OMMT to 275 °C. The hybridized CNCs/OMMT exhibited synergistic effects due to the good affinity through interfacial interactions, resulting in the improvement of the material properties.