There is a huge demand for high-performance materials in extreme environments involving wear and corrosion. High chromium white cast irons (HCWCIs) display better performance than many materials since they are of sufficient hardness for wear protection and can be tailored in chemical compositions to improve corrosion resistance; however, their performance is often still inadequate. This article reviews the chemical composition and microstructure design aspects employed to tailor and develop HCWCIs with combined corrosion and wear resistance. The performance of these alloys under wear and corrosion is reviewed to highlight the influence of these parameters in the industry. Existing challenges and future opportunities, mainly focusing on metallurgical alloy development aspects like chemical composition, casting, and heat treatment design, are highlighted. This is followed by suggestions for potential developments in HCWCIs to improve the performance of materials in these aggressive environments. Many variables are involved in the design to obtain suitable microstructures and matrix composition for wear–corrosion resistance. Computational modeling is a promising approach for optimizing multi-design variables; however, reliable field performance data of HCWCIs in wear–corrosion environments are still inadequate. Quantitative evaluation of the wear–corrosion performance of HCWCIs requires the development of laboratory and field tests using standard conditions like abrasive type and sizes, severity of loading, slurry velocity, pH, and temperature to develop wear–corrosion maps to guide alloy development.