Dielectrophoresis has recently been used for developing high performance elastomer-based structured piezoelectric composites. However, no study has yet focused on the development of aligned thermoplastic-based piezocomposites. In this work, highly anisotropic thermoplastic composites, with high piezoelectric sensitivity, are created. Molten-state dielectrophoresis is introduced as an effective manufacturing pathway for the obtaining of an aligned filler structure within a thermoplastic matrix. For this study, Poly(Ethylene-co Vinyl Acetate) (EVA), revealed as a biocompatible polymeric matrix, was combined with barium titanate (BaTiO₃) filler, well-known as a lead-free piezoelectric material. The phase inversion method was used to obtain an optimal dispersion of the BaTiO₃ within the EVA thermoplastic matrix. The effect of the processing parameters, such as the poling electric field and the filler content, were analyzed via dielectric spectroscopy, piezoelectric characterization, and scanning electron microscopy (SEM). The thermal behavior of the matrix was investigated by thermogravimetric analysis (TGA) and differential scanning calorimetry analysis (DSC). Thermoplastic-based structured composites have numerous appealing advantages, such as recyclability, enhanced piezoelectric activity, encapsulation properties, low manufacturing time, and being light weight, which make the developed composites of great novelty, paving the way for new applications in the medical field, such as integrated sensors adaptable to 3D printing technology.