Electrochemical deposition in alumina templates is proved as a promising method for production of Co(Cu)/Cu nanowires showing high giant magnetoresistance (GMR). This study discusses the deposition of multilayered structures in highly ordered alumina templates in dependence on diffusion (Cu) or kinetically controlled (Co) behavior. Results show a high impact of spherical diffusion on the enhancement of current density of the diffusion controlled component compared to deposition of thin films on planar electrodes. To achieve a separation of the layers and to decrease the amount of Cu in the Co layer the deposition potential of Co was shifted toward more negative potentials. Lithographic structuring of the template surface was carried out to allow a 4-point measurement of the resistance. A high GMR of about 12% was obtained for [Co(Cu) (9 nm)/Cu (11 nm)](380) multilayered nanowires with high accuracy and reproducibility. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.006302jes] All rights reserved.