To obtain high-performance dielectric materials with high dielectric constant and low dielectric loss, novel polymer composites based on poly(arylene ether nitrile) and Ag nanoparticles decorated halloysites nanotube(HNTs) were presented. For this purpose, halloysites nanotubes were modified by bio-inspired polydopamine coating, which acted as both the template and reducing agent for decoration of HNTs by Ag nanoparticles. Moreover, a modified bio-inspired method was developed to realize the surface modification of Ag nanoparticles decorated HNTs hybrid by introducing secondary functional monomer (KH550) to polydopamine system. Therefore, the synergistic effect and good interfacial adhesion contributed to the interesting properties of resulting PEN composites. With addition of 9 wt% Ag nanoparticles decorated HNTs hybrid, the dielectric constant of PEN composite was increased from 3.2 of pure PEN to 10.6 (100 Hz), and low dielectric loss of PEN composite was remained. Furthermore, the tensile strength of PEN composite with 3 wt% of Ag nanoparticles decorated HNTs hybrid increased from 81.07 MPa of pure PEN to 101.3 MPa (increased by 25%). In addition, the glass transition temperature (T-g) reached 171.9 degrees C with addition of Ag nanoparticles decorated HNTs hybrid, which exhibited the significant enhancement in thermal stability. POLYM. ENG. SCI., 58:2227-2236, 2018. (c) 2018 Society of Plastics Engineers