Membrane separation is an effective method for the removal of hazardous materials from wastewater. Halloysite nanotubes (HNTs) were functionalized with 3-aminopropyltriethoxysilane (APTES), and novel polyvinylidene fluoride (PVDF) nanofiltration membranes were prepared by blending with various concentrations of APTES grafted HNTs (A-HNTs). The morphology structure of the membranes were characterized by scanning electron microscope (SEM) and atomic force microscopy (AFM). The contact angle (CA), pure water flux (PWF) and antifouling capacity of membranes were investigated in detail. In addition, the separation performance of membranes were reflected by the removal of dye and heavy metal ions in simulated wastewater. The results revealed that the hydrophilicity of A-HNTs blended PVDF membrane ([email protected]) was enhanced significantly. Owing to the electrostatic interaction between membrane surface and dye molecules, the dye rejection ratio of 3% [email protected] membrane reached 94.9%. The heavy metal ions rejection ratio and adsorption capacity of membrane were also improved with the addition of A-HNTs. More importantly, [email protected] membrane exhibited excellent rejection stability and reuse performances after several times fouling and washing tests. It can be expected that the present work will provide insight into a new method for membrane modification in the field of wastewater treatment.