Aramid macroscale fibers, also called Kevlar fibers, exhibit extremely high mechanical performance. Previous studies have demonstrated that bulk aramid macroscale fibers can be effectively split into aramid nanofibers (ANFs) by dissolution in dimethylsulfoxide (DMSO) in the presence of potassium hydroxide (KOH). In this paper, we first introduced the ANFs into the structure of graphene nanosheets through non-covalent functionalization through π–π stacking interactions. Aramid nanofiber-functionalized graphene sheets (ANFGS) were successfully obtained by adding the graphene oxide (GO)/DMSO dispersion into the ANFs/DMSO solution followed by reduction with hydrazine hydrate. The ANFGS, with ANFs absorbed on the surface of the graphene nanosheets, can be easily exfoliated and dispersed in N-methyl-2-pyrrolidone (NMP). Through a combination of these two ultra-strong materials, ANFs and graphene nanosheets (GS), the resultant ANFGS can act as novel nanofillers for polymer reinforcement. We used the ANFGS as an additive for reinforcing the mechanical properties of poly(methyl methacrylate) (PMMA). With a loading of 0.7 wt% of the ANFGS, the tensile strength and Young's modulus of the ANFGS/PMMA composite film approached 63.2 MPa and 3.42 GPa, which are increases of ∼84.5% and ∼70.6%, respectively. The thermal stabilities of ANFGS/PMMA composite films were improved by the addition of ANFGS. Additionally, the transparencies of the ANFGS/PMMA composite films have a degree of UV-shielding due to the ultraviolet light absorption of the ANFs in the ANFGS.