A study investigated hydrogen permeability in sulfur-cured NBR composites filled with carbon black (CB) and silica, using volumetric analysis across pressures ranging from 1.2 to 92.6 MPa. Both pure NBR and MT CB- and silica-filled NBR exhibited a single sorption mechanism that followed Henry’s law, indicating hydrogen absorption into the polymer chains. In contrast, HAF CB-filled NBR displayed dual sorption behavior, adhering to both Henry’s law and the Langmuir model, which suggests additional hydrogen adsorption at the filler interface. Hydrogen diffusivity in NBR followed Knudsen diffusion at low pressures and bulk diffusion at high pressures. In HAF CB-filled NBR, permeability decreased exponentially with increasing density, while in MT CB- and silica-filled NBR, it declined linearly. The strong polymer-filler interactions in HAF CB significantly influenced permeability. Permeability trends closely correlated with hardness, tensile strength, and density, allowing for the establishment of quantitative relationships between these physical and mechanical properties. These findings indicate that analyzing these properties can predict hydrogen permeability, positioning NBR composites as promising sealing materials for high-pressure hydrogen storage in refueling stations and fuel cell vehicles.