This article addresses the effect of nanocrystalline cellulose (NCC) on the mechanical and thermal properties of polypropylene (PP). A new approach was adopted to produce mechanically improved and thermally stable PP-NCC nanocomposite. This approach involved producing optimized PP-NCC nanocomposite by adding NCC nanoparticles to PP matrix at different concentrations by means of injection molding process. The aim of this work was to find the optimum NCC concentration to enhance the mechanical and thermal properties of the PP matrix. The mechanical and thermal behavior of PP-NCC nanocomposite was studied by performing three-point bend, nanoindentation, differential scanning calorimeter (DSC), thermogravimetric analysis (TGA), scanning electron microscope (SEM), and Fourier transform infrared (FTIR) spectroscopy tests. The results showed that the mechanical properties of strength, modulus, and hardness of the nanocomposites increased with the addition of NCC by 6.5%, 19%, and 150%, respectively. DSC results showed that the addition of NCC to PP does not affect the thermal stability (melting temperature). However, TGA showed that upon inclusion of NCC nanoparticles, the thermal stability of the samples improved compared to pure PP except for the 5% added NCC. This is attributed to the presence of NCC rod-like particles that dissipated heat by generating tortuous paths, as depicted in the SEM results and verified by FTIR results.