The addition of Acridine orange (AO) dye to a polymer blend (80% PVA-20% PVP) enhances its optical, electrical, and radiation attenuation properties, which is a promising approach for polymer applications in nuclear radiation shielding. The effects of acridine orange (AO) dye inclusion on the structure of (PVA- PVP) polymer films, as well as their optic, dielectric, and shielding properties, are studied in this paper. The effect of the Acridine orange (AO) dye on the lattice of the (PVA- PVP) blend is also investigated. With increased AO dye concentration in the UV–Vis range (200–600 nm), UV–Vis absorption spectroscopy shows a greater absorption of the composites. The reduction in hybrid film bandgap due to localized states in the forbidden region makes the current films suitable for optoelectronic, solar cell, and other applications. Composite films have proven to be effective as high-power laser blocking filters in a variety of wavelength ranges. At room temperature, the dielectric constant ε’, dielectric loss ε″ and ac conductivity σac were examined with frequency (100 Hz–1 MHz) and AO dye concentration. The addition of AO dye increases the σac of the (PVA-PVP) blend, which is used in various semiconductor devices. The radiation attenuation qualities were studied using the Phy-X/ PSD program. All radiation shielding characteristics are highly dependent on the density and doping AO dye content in the blend polymeric matrix. Our findings revealed that the rising reinforcement ratio of AO dye has a direct relationship with the analyzed parameters. The preceding investigations into the behavior of doped materials by AO dye have led to the conclusion that AO dye is a useful multifunctional technique that enhances the optical and individual radiation attenuation characteristics of (PVA-PVP) polymers.