The application of bulk metallic glasses (BMGs) as advanced wear-resistant materials has remained limited despite optimistic expectations. In this work, we develop a series of novel Fe-based BMGs with improved wear resistance by altering the Cr and Mo contents in an Fe−Cr− Mo−C−B−Y glass-forming system. Experimental results demonstrate that increasing Cr and Mo contents enhance the thermal stability and hardness (H v ) of the resulting BMGs without reducing their fracture toughness (K c ). The enhanced hardness is mainly attributed to the increased fraction of the stiff (Cr,Mo)−C covalent bonds in the resultant BMGs, as revealed by X-ray photoelectron spectrograph measurement. Worn surface/subsurface observations and stress field modeling reveal the activity of two kinds of wear mechanisms, i.e., hardnesscontrolled abrasion wear and toughness-controlled fatigue wear. We further clarify the enhanced wear performance of the Febased BMGs according to an effective indicator K c 3/4 H v 1/2 that correlates positively with the wear resistance of the samples. The optimal Fe-based BMG sample possessed versatile properties, including a strong glass-forming ability (i.e., a critical diameter of 8 mm), a high hardness of 1335 H v , and a very low specific wear rate of ∼1.3 × 10 −6 mm 3 N −1 m −1 , which represents one of the most outstanding Fe-based BMGs reported thus far.