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Nanoparticles with aerodynamic diameters of less than 100 nm pose serious problems to human health due to their small size and large surface area. Despite continuous progress in materials science to develop air remediation technologies, efficient nanoparticle filtration has appeared to be challenging. This study showcases the great promise of MXene-coated polyester textiles to efficiently filter nanoparticles, achieving a high efficiency of ~90% within the 15–30 nm range. Using alkaline earth metal ions to assist textile coating drastically improves the filter performance by ca. 25%, with the structure–property relationship thoroughly assessed by electron microscopy and X-ray computed tomography. Such techniques confirm metal ions’ crucial role in obtaining fully coated and impregnated textiles, which increases tortuosity and structural features that boost the ultimate filtration efficiency. Our work provides a novel perspective on using MXene textiles for nanoparticle filtration, presenting a viable alternative to produce high-performance air filters for real-world applications.