AbstractDiscovery of new magnets with high magnetization has always been important in human history because it has given birth to powerful motors and memory devices. Currently, the binary alloy Fe3Co1 exhibits the largest magnetization of any stable alloys explained by the Slater-Pauling rule. A multi-element system is expected to include alloys with magnetization beyond that of Fe3Co1, but it has been difficult to identify appropriate elements and compositions because of combinatorial explosion. In this work, we identified an alloy with magnetization beyond that of Fe3Co1 by using an autonomous materials search system combining machine learning and ab-initio calculation. After an autonomous and automated exploration in the large material space of multi-element alloys for six weeks, the system unexpectedly indicated that Ir and Pt impurities would enhance the magnetization of FeCo alloys, despite both impurity elements having small magnetic moments. To confirm this experimentally, we synthesized FexCoyIr1-x-y and FexCoyPt1-x-y alloys and found that some of them have magnetization beyond that of Fe3Co1.