The solution casting approach was used to successfully manufacture polyvinylidene fluoride-barium titanate (PVDF-BT) films doped with varied ratios of polyaniline (PANI) (0, 0.5, 1, 2% wt.). The structural and dielectric properties of different prepared films and a selected film irradiated with 0, 10, 20, and 30 kGy from an electron beam accelerator (EB) are investigated. Incorporating PANI into PVDF-BT resulted in a higher β-phase, as evidenced by XRD and FTIR. Besides the amorphization of BT particles inside the irradiated film, EB induces the transition of α-phases into β-phases. Adding PANI, the dielectric constant (ε`) and loss tangent (tanδ) of the PVDF-BT composites increased. In contrast, EB irradiation causes a reduction of ε`and tanδ values of the irradiated sample. Because of the reduced polarization level, the ac conductivity (σac) rose with increasing PANI content in PVDF-BT composite, but it decreased with increasing EB doses. Furthermore, adding PANI to PVDF-BT composite and irradiating with EB generated structural alterations in the material. Incorporating PANI into PVDF-BT and EB irradiation decreased mobile ions and lattice strain inside samples.