Ferroelectric composite structures of poly (vinylidene fluoride-co-trifluoroethylene)/ barium titanate (PVDF-TrFE/BTO) were prepared using a solvent casting method and altered using electrical and mechanical modes to improve their ferroelectric characteristics. The PFM and P-E loop analytic studies validated the enhanced ferroelectric and piezoelectric capabilities of the modified composite structures following mechanical stretching and electrical poling. The stretched and poled samples (PT-BT-s-p) were able to achieve a maximum saturated polarization of 5.98 µC/cm2 with suitable saturation loops and domain switching points. The presence of ferroelectric domains was further confirmed by the PFM amplitude and PFM phase graphs of the PT-BT-s-p composite structures. Furthermore, the suggested composite structure achieved a maximum piezoelectric coefficient (d33) value of 11 pC/N. Finally, a lab-scale experiment with a sound wave sensing application was performed and seen with superior outcomes with varying waveforms, amplitudes, and frequencies, making it a promising contender for future sensory devices.