The aim of this study was to produce bulk nanocrystalline Al/Al12(Fe,V)3Si alloys by mechanical alloying (MA) and subsequent hot pressing (HP) of elemental powders. A nanostructured Al-based solid solution was formed by MA of elemental powders for 60 h. After HP of the as-milled powders at 550°C for 20 min, the Al12(Fe,V)3Si phase was precipitated in a nanocrystalline Al matrix. Scanning electron microscopy (SEM) images of the bulk samples represented a homogeneous and uniform microstructure that was superior to those previously obtained by rapid solidification–powder metallurgy (RS–PM). Nanostructured Al?8.5Fe?1.3V?1.7Si and Al?11.6Fe?1.3V?2.3Si alloys ex-hibited high HV hardness values of~205 and~254, respectively, which are significantly higher than those reported for the RS–PM counter-parts.