The applicability of the strain-induced bcc phase of Co in magnetoresistive devices was studied. Ultrathin bcc Co͑001͒ films and the influence of the additional layers needed for magnetoresistive devices were examined by means of 59 Co nuclear magnetic resonance ͑NMR͒. NMR is shown to be a discriminating technique for determining the presence of structurally and magnetically pure bcc Co. The maximum stability for uncovered and Fe-covered layers grown on Fe͑001͒/GaAs͑001͒ and Fe͑001͒/Ge͑001͒ seed layers is found to be about 2 nm. Growth of an Al 2 O 3 top layer preserves the bcc phase, in contrast to a Cu film which causes a transformation of the bcc structure to the fcc or the hcp phase. The bcc-preserving effects of Al 2 O 3 imply the possibility to fabricate magnetic tunnel junctions with bcc Co͑001͒ bottom electrodes. Although bcc Co is a force-induced structure, thin layers are shown to be stable over a few years when Al 2 O 3 has been grown on top. Junction structures using bcc Co͑001͒ bottom electrodes were grown and characterized.