Nanocomposite membranes containing poly(m-phenylene isophthalamide) (PMIA) and organically modified montmorillonite (OMMT) were prepared by a combination of solution dispersion and wet-phase inversion methods, and the effects of OMMT addition on the properties and performance of fabricated nanofiltration membranes were investigated. The membranes were characterized by contact angle measurements, scanning electron microscopy (SEM), atomic force microscopy (AFM), thermogravimetric analysis, and zeta potential.The performance of the membranes was elucidated by the removal of perfluorooctane sulfonate (PFOS) at neutral pH. Increasing OMMT concentration improved the thermal stability and hydrophilicity of the membranes. The permeation and rejection of PFOS were significantly improved. The performance of fabricated nanofiltration membranes in removal of PFOS varied depending on the solute and membrane properties as well as solution conditions. Finally, a comparison between fabricated membranes and a commercial NF membrane (ESNA1-K1, Hydecanme) proved that the OMMT addition is a convenient procedure for producing nanocomposite membranes with superior properties and performance.