The present study introduces a novel attempt in enhancing the performance of triboelectric nanogenerators (TENGs) by incorporating one-dimensional functionalized multi-walled carbon nanotubes (FMWCNTS) into the polymer matrix to employ as a tribopositive layer. This study systematically investigates the influence of FMWCNTS concentration, external force frequency, and applied force on the electrical output of the FMWCNTS:TENGs, providing valuable insights into optimizing their performance for various applications. The results showed the FMWCNTS:TENGs exhibited significant improvement in electrical output compared to pristine PVA-TENGs, with an optimal FMWCNTS concentration of 2.00   mL yielding the highest voltage of 354.53   V and current of 17.63   µA, respectively. The device also exhibited excellent electrical stability and mechanical durability over 12,000 cycles of operation. The results highlight the potential of FMWCNTS in improving the triboelectric properties of TENGs, making them promising contenders for self-powered applications, including wearable electronics, sensors, and ambient energy harvesting.