Flexible polymer-based composites exhibiting high dielectric constant as well as low dielectric loss have been intensively investigated for their potential utilization in electronics and electricity industry and energy storage. Resulting from the polar -CN on the side chain, polyarylene ether nitrile (PEN) shows relatively high dielectric constant which has been extensively investigated as one of the hot spots as dielectric materials. However, the dielectric constant of PEN is still much lower than the ceramic dielectrics such as BaTiO 3 , TiO 2 , and Al 2 O 3 . In this review, recent and in-progress advancements in the designing and preparing strategies to obtain high-k PEN-based nanocomposites are summarized. According to the types of the added fillers, the effects of organic fillers, dielectric ceramic fillers, and conductive fillers on electric properties of PEN-based composites are investigated. In addition, other factors including the structures and sizes of the additive, the compatibility between the additive agent and the PEN, and the interface which affects the dielectric properties of the obtained composite materials are investigated. Finally, challenges facing in the design of more effective strategies for the high-k PEN-based dielectric materials are discussed.