This work investigates the isolation of cellulose nanocrystals (CNC) from sugarcane bagasse (SCB) waste and the evaluation of their mechanical reinforcement capability for k-carrageenan biopolymer. The results from Atomic Force Microscopy and Transmission Electron Microscopy indicated the successful extraction of CNC from SCB following alkali, bleaching and acid hydrolysis treatments. The CNC displayed a needle-like structure with an average aspect ratio of 55. The surface functionality of the CNC was evaluated by Fourier Transform Infrared Spectroscopy and X-ray Photoelectron Spectroscopy measurements. X-ray diffraction studies showed that the as-extracted CNC exhibit cellulose I crystalline structure, with a crystallinity index of 80%. The obtained CNC were dispersed into k-carrageenan biopolymer matrix at various CNC contents (1, 3, 5 and 8 wt%) and the prepared films were further characterized. The incorporation of CNC decreased the light transmittance values but enhanced the mechanical properties compared with the neat k-carrageenan film. Empirical Halpin-Tsai model was used to predict the CNC dispersion within k-carrageenan matrix. The obtained nanocomposite films have the potential to be used as food packaging material.