Superior abrasive wear resistance, combined with relatively low production costs, makes high Cr white cast irons (WCIs) particularly attractive for applications in the grinding, milling, and pumping apparatus used to process hard materials. Hypoeutectic, eutectic, and hypereutectic cast iron compositions, containing either 15 or 26 wt pct chromium, were studied with respect to the macrostructural transitions of the castings, solidification paths, and resulting microstructures when poured with varying superheats. Completely equiaxed macrostructures were produced in thick section castings with slightly hypereutectic compositions. High-stress abrasive wear tests were then performed on the various alloys to examine the influence of both macrostructure and microstructure on wear resistance. Results indicated that the alloys with a primarily austenitic matrix had a higher abrasion resistance than similar alloys with a pearlitic/bainitic matrix. Improvement in abrasion resistance was partially attributed to the ability of the austenite to transform to martensite at the wear surface during the abrasion process.