This study explores the fabrication of electret nonwoven structures for high-efficiency air filtration, utilizing the blow spinning technique. In response to the growing need for effective filtration systems, we aimed to develop biodegradable materials capable of capturing fine particulate matter (PM2.5) without compromising environmental sustainability. Polylactic acid (PLA) was used as the primary polymer, with the addition of SiO2 and MoS2 to enhance the fibers’ charge retention and filtration performance. The fibers were charged electrostatically to improve particle capture efficiency. The experimental results showed that fibers containing 5% MoS2 exhibited the highest filtration efficiency, surpassing those with SiO2, despite MoS2 being a semiconductor and SiO2 a dielectric. Furthermore, the addition of MoS2 improved the filtration efficiency across a range of particle sizes (0.2–1 µm) while maintaining a manageable pressure drop. These findings suggest that incorporating MoS2 in electret nonwoven structures can significantly improve filtration performance, making it a promising material for advanced air filtration applications. This study contributes to the development of eco-friendly filtration materials with high performance, essential in reducing exposure to airborne pollutants.