This study presents functionalized carbon nanotubes (CNTs) decorated with functionalized barium titanate (BT) (denoted as BT@CNTs) via hydrothermal and self-assembly methods to improve dispersion in polypropylene (PP) matrix with enhanced thermal, mechanical, and thermomechanical properties. The CNTs, BT, and BT@CNTs with the addition of polypropylene maleic anhydride (PPMA) compatibilizer were used in the fabrication of the PP based nanocomposites for this study via solution mixing and melt compounding. FTIR, TEM, and SEM analyses, respectively revealed that the nanoparticles were successfully functionalized, CNTs decorated with BT, and well dispersion in the PP matrix. PP/BT@CNTs-based nanocomposite showed optimal tensile strength, modulus, heat deflection, and thermal stability of about 16.8%, 26.5%, 20.1%, and 30oC higher than that obtained for the pure PP. These properties were also respectively 10.6%, 17.6%, 19.0%, and 5.0oC higher than PP/3CNTs nanocomposite when compared to PP/3BT@CNTs. The PP/BT@CNTs based nanocomposites also revealed enhanced dynamic mechanical properties. The better performance in the measured properties of PP/BT@CNTs compared to pure PP and PP/CNTs were attributed to their uniform microstructures, effective interlocking of the PP matrix due to the presence of BT on CNTs surfaces.