Using a cold graphite mold casting method, bulk AlNiY chill-zone alloys were prepared at hypereutectic compositions with Al content from 85 at.% to 94 at.%. It was found that ultra-hard surface layers with a thickness of about 200 μm and submicron grain size form when the melt can be undercooled without heterogeneous nucleation at the mold contact surface. This hard chill-zone forming in contact with the mold possesses Vickers microhardness Hv about 350–420 and is thus harder than fully amorphous Al alloys. In compression, ultimate strength more than 1.1 GPa and true strain more than 150% without failure were achieved simultaneously. The combination of high strength and good plasticity will be discussed in relation to the special structure of the chill-zone alloy.