Polymeric gradient film consisting of the plastic nanoparticles in addition to an elastomer matrix was created by driving the charged sulfonated polystyrene (PS) nanoparticles in polydimethylsiloxane (PDMS) matrix under direct‐current electric field. The gradient morphology was frozen by thermal curing. The morphology, composition, damping, and mechanical properties of cured PS/PDMS gradient film containing 10 wt % of PS nanoparticles were measured with scanning electron microscopy, energy‐disperse spectroscopy, and dynamic thermal mechanic analysis and tensile test, respectively. In comparison with the isotropic PS/PDMS film, the gradient film shows a better damping property, and a higher tensile strength and elongation at breaking. The interpretation in terms of deformation and fracture mechanism of gradient structure was proposed. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2020, 137, 48401.