Metallic glasses (MGs) with the unique long-range disordered and short-range ordered atomic structure have attracted extensive attention in the field of environmental catalysis due to their advanced catalytic capability. Herein, CuZr-based MGs are first proven to exhibit superior catalytic performance toward the degradation of organic pollutants compared to the annealed ribbons with different crystal structures; many Cu nanocomposites are gradually in situ precipitated on the surface of the ribbons. The enhanced catalytic behavior is mainly attributed to the random atomic packing structure accelerating electron transport and providing sufficient active sites. On the other hand, the active species, for example, ·OH, ·O