Methanation is a classical reaction in heterogeneous catalysis and significant effort has been put into improving the industrially preferred nickel-based catalysts. Recently, a computational screening study showed that nickel-iron alloys should be more active than the pure nickel catalyst and at the same time less expensive. This was previously verified experimentally for pure CO hydrogenation. In this study, the improved activity is also verified for CO2 hydrogenation as well as for simultaneous CO and CO2 hydrogenation. Author Keywords: CO and CO2 hydrogenation; volcano-plot; computational screening; Pareto plot; Ni-Fe bimetallic catalysts