Al-rich 94Al–6Mn and 94Al–4Mn–2Fe alloys were suction-cast to evaluate the feasibility of obtaining bulk quasicrystal-strengthened Al-alloys at intermediate cooling rates alloyed with non-toxic, easily accessible and affordable additions. The influence of different cooling rates on the potential formation of a quasicrystalline phase was examined by means of scanning and transmission electron microscopy, X-ray diffraction and differential scanning calorimetry. Increased cooling rates in the thinnest castings entailed a change in sample phase composition. The highest cooling rates turned out to be insufficient to form an icosahedral quasicrystalline phase (I-phase) in the binary alloy. Instead, an orthorhombic approximant phase occurred (L-phase). The addition of Fe to the 94Al–6Mn binary alloy enhanced the formation of a quasicrystalline phase. At intermediate cooling rates of 10²–10³ K/s, various metastable phases were formed, including decagonal and icosahedral quasicrystals and their approximants. Rods (1 mm in diameter) composed of I-phase particles embedded in Al matrix exhibited a hardness of 1.5 GPa, much higher than the 1.1 GPa of 94Al–6Mn.