Design and fabrication of bimodal structures are essential for successful development of advanced air filters with ultralow airflow resistance. To realize this goal, simplified processing procedures are necessary for meeting the practical needs. Here, a bimodal protein fabric with high-performance air filtration, and effectively lowered airflow resistance is reported. The various functional groups of proteins provide versatile interactions with pollutants. By utilizing a novel and cost-effective "cross-axial" configuration with an optimized condition (75° of contacting angle between solution nozzle and cospinning solvent nozzle), the diffusion in Taylor cone is in situ controlled, which results in the successful production of bimodal protein fabric. The bimodal protein fabric (16.7 g/m2 areal density) is demonstrated to show excellent filtration performance for removing particulate matter (PM) pollutants and only causes 17.1 Pa air pressure drop. The study of multilayered protein fabric air filters shows a further improvement in filtration performance of removing 97% of PM0.3 and 99% of PM2.5 with a low airflow resistance (34.9 Pa). More importantly, the four-layered bimodal protein fabric shows an exceptional long-term performance and maintains a high removal efficiency in the humid environment. This study presents an effective and viable strategy for fabricating bimodal fibrous materials for advanced air filtration.