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The reactive metal-support interaction in the Cu-In 2 O 3 system and its implications on the CO 2 selectivity in methanol steam reforming (MSR) have been assessed using nanosized Cu particles on a powdered cubic In 2 O 3 support. Reduction in hydrogen at 300 °C resulted in the formation of metallic Cu particles on In 2 O 3 . This system already represents a highly CO 2 -selective MSR catalyst with ~93% selectivity, but only 56% methanol conversion and a maximum H 2 formation rate of 1.3 µmol g Cu −1  s −1 . After reduction at 400 °C, the system enters an In 2 O 3 -supported intermetallic compound state with Cu 2 In as the majority phase. Cu 2 In exhibits markedly different self-activating properties at equally pronounced CO 2 selectivities between 92% and 94%. A methanol conversion improvement from roughly 64% to 84% accompanied by an increase in the maximum hydrogen formation rate from 1.8 to 3.8 µmol g Cu −1  s −1 has been observed from the first to the fourth consecutive runs. The presented results directly show the prospective properties of a new class of Cu-based intermetallic materials, beneficially combining the MSR properties of the catalyst's constituents Cu and In 2 O 3 . In essence, the results also open up the pathway to in-depth development of potentially CO 2 -selective bulk intermetallic Cu-In compounds with well-defined stoichiometry in MSR.