Bulk metallic glasses are modern engineering materials with unique functional properties. Zr-based alloys are particularly attractive as they exhibit high glass forming ability as well as good mechanical properties. Due to their relatively high thermal stability, reaching as much as 400 °C, they can be surface-treated in low-temperature plasma to further improve their mechanical properties. The subject of this study was to determine the influence of the technological parameters of nitriding in low-temperature plasma on the structure and mechanical properties of Zr48Cu36Al8Ag8 bulk metallic glass. In the course of this study, the influence of the ion accelerating voltage on the structure and micromechanical properties of the bulk metallic glass was analyzed. The produced samples were characterized in terms of nanohardness, layer adhesion by using the scratch test, and wear resistance by using the ball-on-disc method. As a result of low-temperature plasma nitriding, a significant increase in the surface nanohardness of the Zr48Cu36Al8Ag8 bulk metallic glass was obtained. The produced layers exhibited high adhesion to the substrate and they improved the wear resistance of the glass. The present study indicates the possibility of modifying the surface properties of bulk metallic glasses by using diffusion processes in low-temperature plasma without substrate crystallization.