Regenerated cellulose (RC)-based composites reinforced with multi-walled carbon nanotubes (MWCNTs) were prepared by a facile casting method. The morphology and microstructure of the fabricated composites were characterized using transmission electron microscopy, Fourier transform infrared spectroscopy (FTIR) and Raman spectroscopy. Thermogravimetry and derivative thermogravimetric analysis were conducted to investigate the effect of MWCNTs on the thermal behaviors of the RC. The results showed that the introduction of MWCNTs enhanced the thermal stability of the RC. Moreover, the effect of the dispersion state of MWCNTs in microcrystalline cellulose/ZnCl2 solutions with varying MWCNT loadings was studied by rheological tests. The mechanical properties of composite films were remarkably improved compared to those of pure RC film. Specifically, the composite film containing 3 wt% of MWCNTs exhibits a 123% enhancement in tensile strength and a 163% enhancement in the Young's modulus compared with the pure RC film.