Polymer nanofibers have established a robust foundation and possess immense potential in various emerging fields such as sensors and biotechnology. In this study, aqueous dispersions of aramid nanofibers (ANFs) were successfully prepared by using tannic acid (TA). Morphological analysis revealed that TA effectively prevented self-aggregation of ANFs, and preserved the nanofiber structure during TA-assisted solvent exchange. Subsequently, the ANF and TA/ANF films were fabricated using casting and vacuum-assisted filtration techniques. Notably, the tensile strength of the casting TA/ANF film reached 393.8 MPa, exhibiting a remarkable improvement of 41.3% compared to that of the pure ANF film. These exceptional mechanical properties can be attributed to the well-dispersed nanostructures, hydrogen-bonding interactions, zigzag structures, and fiber-bridging effects. Furthermore, the TA/ANF film demonstrated superior ultraviolet (UV) shielding capabilities, visible transparency properties, and excellent resistance to chemical reagents. The above-mentioned interesting findings demonstrate its potential as a nanofiber-reinforced material for poly(vinyl alcohol) (PVA) composites.