Co–Fe films are grown onto plane pre-treated Cu foils; the effects of the alloy composition on the morphology and the crystal texture of the electrodeposited films and their anisotropic magnetic hysteresis properties are explored. Nucleation and crystallization mechanisms in these Co-rich layers are also investigated with pulse-reverse plating techniques, using the first cathodic pulse current–time transients. In the diffusion controlled regime the deposition mechanism is found to involve progressive nucleation with three-dimensional (3D) growth, except for the equiatomic Fe50Co50 solution where nucleation tends to become instantaneous. The different morphologies and size scales observed are described and correlated with coercivity. The films are electrodeposited onto electrochemically pre-treated Cu substrates from feeds of nominal Fe/Co mol ratios between 0/100 and 50/50. The composition of the deposited layers, as determined by energy dispersive X-ray spectroscopy, are quite close to the nominal values. Cyclic voltammetry determinations exhibit only a single reduction process on the cathode, indicating that a unique (Co100−xFex) phase grows. Depending on composition and on the substrate pre-treatment, these layers exhibit textures with features of different sizes. X ray diffraction patterns indicate that the nanostructures with Fe contents above 20at.% crystallize in a body-centered cubic cell, while samples with Fe contents below this value are fcc. Regarding the effect of composition on the morphology, Co and Co-rich layers are compact, with large (100–300nm) agglomerates of quite equiaxed, densely packed particles (average 50nm); as the iron content increases above 15at.%, faceted particles 100nm in size are observed. All the electrodeposited layers are soft ferromagnetic at room temperature, with an in plane easy axis; coercive fields/forces between 10mT and 71mT are measured at 300K.