Chromium containing metals are an industry staple due to unparalleled corrosion resistance and durability. Unfortunately, many if not all Cr-containing alloys can produce Hexavalent Chromium (Cr6+), a known carcinogen [1,2]. Studies conducted by the California Air Resources Board (CARB) showed that 30-60 percent of chromium emissions produced in thermal spray processing can contain Cr6+ . In addition, several independent studies found that Cr6+ emissions produced from Twin Wire Arc Spray (TWAS) can be up to 3,000 times greater than the legal limits established by the CARB. This study details efforts to develop the next generation of high performance thermal spray alloys which are Chromium free, thereby resulting in zero Cr6+ emissions. In order to meet these objectives high throughput computational metallurgy was employed. The initial results have shown that next generation alloys can be developed to meet or exceed the performance of incumbent Cr-bearing alloys currently in service, and that the future of Cr-free alloys is on the horizon.