The quasicrystalline structures of alloys with nominal compositions of Al72Ni13.4Co14.6 and Al72.3Ni7.8Co19.8 were characterized by X-ray diffraction, transmission electron microscopy and scanning electron microscopy. For catalytic application, the solids were leached with an alkaline NaOH solution and tested at 373 K with two model reactions under atmospheric pressure: hydrogenation of crotonaldehyde and acetonitrile. The catalytic activities of these leached alloys were compared to that of a Raney nickel reference catalyst. Catalysts prepared from quasicrystals showed high catalytic activities and high selectivities towards butanal (in crotonaldehyde hydrogenation) and ethylamine (in acetonitrile hydrogenation).