All-cellulose nanocomposite films were prepared using native cellulose nanofibrils (CNFs) as fillers and lithium chloride/N,N-dimethylacetamide (LiCl/DMAc) dissolved regenerated cellulose as the matrix. The CNFs, with diameters in the range of 15–40nm were obtained by combined physical methods of ultrasonic treatment and high shear homogenization. The morphology, structure, and properties of the nanocomposite films were characterized by scanning electron microscope (SEM), X-ray diffraction (XRD), optical transmittance, thermal gravimetric analysis (TGA), and mechanical testing. The nanocomposite films exhibited good optical transparency, thermal stability, and remarkably enhanced mechanical properties compared to the regenerated cellulose matrix. By varying the CNFs content, the tensile strength of the nanocomposite films increased from 61.56MPa to 99.92MPa and the Young's modulus increased from 0.76GPa to 4.16GPa. This work provided a promising pathway for manufacturing high performance and environmental-friendly all-cellulose nanocomposites.