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Novel polyimide/γ-ray irradiated MWCNTs (PI/γ-MWCNTs) nanocomposites with improved dielectric properties were fabricated by casting and curing processes. The interfacial interactions between the two domains, i.e. PI and MWCNTs, were enhanced by hydrogen bonding between the hydroxyl groups present on PI and modified CNTs. A PI matrix having pendant phenolic hydroxyl groups was derived from pyromellitic dianhydride (PMDA) and diamine monomer 4,4′-diamino-4′′-hydroxytriphenylmethane. MWCNTs (5-20 wt%) were dispersed in the synthesized PI matrix. Before addition to PI, the surface of MWCNTs was equipped with hydroxyl and carboxylic groups by irradiating with γ-rays under a dry oxygen environment. Surface examination of PI/γ-MWCNTs composite films by scanning electron microscopy (SEM) revealed that MWCNTs are uniformly dispersed and completely wrapped by PI matrix, most likely due to the hydrogen bonding. The influence of greater adhesion of MWCNTs with PI matrix on the dielectric, visco-elastic, and mechanical properties of final PI/γ-MWCNTs nanocomposites was explored using appropriate analytical techniques. The composite films exhibited high dielectric constant, a 7.6 folds improvement as compared to pristine PI. The storage modulus (E′) and glass transition temperature (Tg) demonstrated an improvement of 1.4 and 1.2 folds, respectively. Similarly, mechanical and thermal properties were also found to be improved remarkably. We believe that significant property enhancement of PI/γ-MWCNTs nanocomposites is the direct consequence of increased interface compatibility via hydrogen bonding between polymer matrix and carbon nano-filler.