In the modern era, the invention of new energy sources is important in order to make advances possible in electronic media. A triboelectric nanogenerator (TENG) is considered to be strong design that converts mechanical power into electrical power, using organic (polymer) or inorganic (lead, ceramic etc) materials to initiate the triboelectrification process, followed by charge separation. In this study, a lead-free BaTiO3/PDMS-Al-based TENG was fabricated by mixing tetragonal ferroelectric BaTiO3 nanocrystals in a PDMS matrix to make a composite for a working electrode film. It is worth noting that a new post- poling process has been introduced to align the dipole structures in the BaTiO3 nanocrystals, and to attain a high electron density on the surface of the working electrode film. The output was recorded up to 375 V and 6 μA of close circuit voltage and short circuit current, respectively, at a current density of 0.3 μA cm-2 and an effective power equal to 2.25 mW at a load resistance of 100 MΩ, and is four times higher than a PDMS-Al-based TENG. This study also reveals the hidden locks that will enable other inorganic materials with a dipole structure to enhance their output using the post-poling technique. The TENG has a vast field of applications due to its stability, the flexibility of its thin films and its biocompatibility. It is also an aid for exploring new TENG devices with enhanced output performance.