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By means of impact abrasion tests, micro-hardness tests, and worn surface morphology observation via SEM, a comparison research based upon different impact abrasive wear conditions was conducted in this research to study the influence of different carbon contents (1.25wt.%, 1.35wt.%, and 1.45 wt.%) on the wear resistance and wear mechanism of water-quenched Mn13Cr2 and Mn18Cr2 cast steels. The research results show that the wear resistance of the Mn18Cr2 cast steel is superior to that of the Mn13Cr2 cast steel under the condition of the same carbon content and different impact abrasive wear conditions because the Mn18Cr2 cast steel possesses higher worn work hardening capacity as well as a more desirable combination of high hardness and impact toughness than that of the Mn13Cr2 cast steel. When a 4.5 J impact abrasive load is applied, the wear mechanism of both steels is that plastic deformation fatigue spalling and micro-cutting coexist, and the former dominates. When the carbon content is increased, the worn work hardening effect becomes increasingly dramatic, while the wear resistance of both steels decreases, which implies that an increase in impact toughness is beneficial to improving the wear resistance under severe impact abrasive wear conditions. Under the condition of a 1.0 J impact abrasive load, the wear mechanism of both steels is that plastic deformation fatigue spalling and micro-cutting coexist, and the latter plays a leading role. The worn work hardening effect and wear resistance intensify when the carbon content is increased, which implies that a higher hardness can be conducive to better wear resistance under low impact abrasive condition.