Polycyclic aromatic hydrocarbons (PAHs) are persistent organic pollutants that may contaminate various water sources and pose serious dangers to human health and the environment. Due to their capacity for size-based separation, nanofiltration membranes have become efficient instruments for PAH removal. However, issues such as membrane fouling and ineffective rejection still exist. To improve PAH rejection while reducing fouling problems, this work created a new gradient crosslinking poly(vinylpyrrolidone) (PVP) nanofiltration membrane. The gradient cross-linking technique enhanced the rejection performance and antifouling characteristics of the membrane. The results demonstrated that the highest membrane flow was achieved at a 0.15% SDS-PVP membrane. There is a trade-off between membrane flux and salt rejection since salt rejection increases with SDS owing to the growth of big pores. The membrane flux was reduced for the 0.25% SDS-PVP membrane owing to poor SDS dispersion. The prepared membrane showed enhanced removal efficiencies for the removal of the PAH compounds. The PVP membrane has the potential to be used in several water treatment applications, improving water quality, and preserving the environment.