Most metals and alloys suffer from high friction and wear due to their low hardness and lack of self-lubrication. Although plenty of strategies have been proposed, it is still a long-standing challenge to achieve diamond-like wear in metals. Metallic glasses (MGs) are supposed to possess low coefficient of friction (COF) because of their high hardness and fast surface mobility. However, their wear rate is larger than that of diamond-like materials. Here, this work reports the discovery of Ta-rich MGs that exhibit diamond-like wear. This work develops an indentation approach for high-throughput characterization of crack resistance. By employing deep indentation loading, this work is able to efficiently identify the alloys that exhibit better plasticity and crack resistance according to the differences of indent morphology. With high temperature stability, high hardness, improved plasticity, and crack resistance, the discovered Ta-based MGs exhibit diamond-like tribological properties, featured by COF as low as ≈0.05 for diamond ball test and ≈0.15 for steel ball test, and specific wear rate of only ≈10 −7 mm 3 N −1 m −1 . The discovery approach and the discovered MGs exemplifie the promise to substantially reduce friction and wear of metals and may unleash the potential of MGs in tribological applications.