The grephene (GE)@waterborne polyurethane (WPU) microcapsule (GE@WPU) is synthesized and introduced GE@WPU microcapsules to aramid fibers (AF) surface. Compare with GE is directly added to WPU solution, the GE@WPU microcapsule suspension is improved significantly. The results show that the tensile strength (19.1 cN/dtex) of modified AF is higher than unmodified AF (17.5 cN/dtex), the elongation at break (1.47%) of modified AF is lower than the unmodified AF (1.51%); the GE@WPU microcapsules can significantly decrease the surface resistivity. Modified AF is introduced into natural rubber (NR), findings indicated that the GE@WPU microcapsule modified AF contribute to enhancing the interfacial adhesion properties of AF/NR composites, the pull-out force of modified AF/NR composites is increased with the content of GE@WPU microcapsules increase, the pull-out force (142 N/cm) of modified AF/NR composites is higher than the unmodified AF/NR composites (64 N/cm). This means that the method can be applied in the fiber-reinforced composites. [GRAPHICS]