ZnMg oxide tunnel barriers are grown which, when sandwiched between ferri- or ferromagnetic layers, form magnetic tunnel junctions exhibiting high tunneling magnetoresistance (TMR). The TMR may be increased by annealing the magnetic tunnel junctions. The zinc-magnesium oxide tunnel barriers may be incorporated into a variety of other devices, such as magnetic tunneling transistors and spin injector devices. The ZnMg oxide tunnel barriers are grown by first depositing a zinc and/or magnesium layer onto an underlying substrate in oxygen-poor (or oxygen-free) conditions, and subsequently depositing zinc and/or magnesium onto this layer in the presence of reactive oxygen.