The mechanical properties of Zn–4 wt% Al casting alloys are compared after various processing methods including sand casting, die-casting, and high energy cryogenic ball milling. For the cast structures there is an increase in strength when transitioning from a coarse sand casting microstructure to a finer grained thin-section die-casting. This is in contrast to a decrease in strength and increase in ductility seen when the cast structure is broken up by high energy cryogenic ball milling to a uniform ultra-fine grain scale. The ultra-fine grained structures produced by cryogenic ball milling subjected to a range of isothermal heat treatments follow the Hall–Petch behavior over the range of grain sizes studied.