Dielectric elastomers with conducting inorganic fillers offer a wide range of uses, including capacitive energy storage, elastomer sensors, actuators, and many more. In this approach, low dielectric loss and high dielectric constant may be made possible by ternary composites that use metal alloy components as reinforcing fillers. Here, Cu-based alloy was added to acrylonitrile-butadiene rubber (NBR) to produce ternary rubber composites. Unfortunately, the Cu–Al–Zn alloy’s material incompatibility with the rubber matrix typically leads to phase separation, void formation, and particle aggregation, all of which have a dramatic negative impact on performance. Using 3-(trimethoxysilyl)propyl methacrylate as a coupling agent, Cu–Al–Zn alloy particles were uniformly dispersed onto the NBR rubber matrix through surface modification. By using scanning electron microscopy, the appropriate reinforcement of modified Cu-based alloy particles into NBR was carefully examined. The effect of modified Cu–Al–Zn alloy loading on the swelling behavior of the composite was also investigated. The findings show that the shape and dispersion state of modified Cu–Al–Zn alloy were important for the dielectric characteristics of the NBR compounds. By adding reinforced modified Cu-based alloy to the NBR matrix, mechanical characteristics were significantly improved. The uniform dispersion of modified Cu–Al–Zn alloy particles and strong interfacial compatibility with rubber matrix are the reasons for the outstanding performance of NBR composites, which suggests high-performance dielectric composite.