Aramid pulp/fiber is the most vital ingredient of brake friction material (FM) formulation. It is perpetually added to achieve quality brake pads/shoes and improve the overall friction and wear performance. Additionally, novel Zylon fibers have a superior property to aramid fibers. However, no studies give insights on their influence on brake noise and vibration (NV) performance. In the current work, a series of six different types of eco-friendly brake pads was developed. The first five contain aramid pulp, aramid short fibers, and Zylon fibers of different sizes (1, 3, and 6 mm) as the theme ingredients (3 wt %) by keeping the parent composition identical. Additionally, one more pad was developed that contains no aramid/Zylon fibers (i.e., reference pad). The pads were characterized for physical and mechanical properties. The damping and natural frequencies of pads were measured experimentally and numerically. All brake pads were evaluated for detailed NV performance by following the SAE J 2521 test schedule. In addition, numerical simulation was performed to validate the experimental brake squeal results. Results revealed that aramid/Zylon fiber-based pads improved the porosity, damping, and compressibility. Overall, brake noise and vibrations were improved for aramid/Zylon fiber-based pads by 1.2–1.5 dBA and 20–25%, respectively, compared to the reference pad. The complex eigenvalue analysis (CEA) proved that squeal was mainly influenced by the damping and density of the pad materials. Thus, aramid/Zylon fiber-based pads can effectively suppress the instability of the brake system and reduce the brake squeal propensity.