Poly (arylene ether nitrile)/fullerene (PEN/fullerene) nanocomposites were prepared by a facile solution-cast method and the rheological, dielectric, mechanical, and morphological properties of the resulted nanocomposites were systematically studied and compared. Rheological studies showed PEN/fullerene nanocomposites percolation network formed at fullerene containing of 1.50 wt %, when the shear frequency was fixed at 0.1 Hz, the fitted rheological percolation threshold was about 1.55 wt %, very close to the experimental observations. The dielectric transaction occurs when the fullerene loading reached 1.50 wt %, that is very close to its rheological percolation threshold. At this point, PEN/fullerene nanocomposites also showed the optimal mechanical properties with a tensile strength of 93.6 MPa and modulus of 1951.5 MPa, which is increased by 27% and 15% compared with the pure PEN. SEM and TEM images have manifested the separate fullerene aggregated to fullerene bundles in PEN/fullerene nanocomposites, and the dispersion of fullerene bundles begin to go bad when the containing above 1.50 wt %. The PEN/fullerene nanocomposites can be widely used due to its excellent dielectric and mechanical performance. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 40100.