The synthesis of materials and the studies of crystal structure and 57 Fe Mössbauer effect were performed for Tb0.27Dy0.73(Fe1−xCox)2 intermetallics. Terfenol-D (Tb 0.27Dy0.73Fe2) is the starting compound of this Fe/Co-substituted series. X-ray measurements showed evidence of a pure cubic Laves phase C15, MgCu2-type, and unit cell parameters were determined across the series. A Co substitution introduced local area, at sub-nanoscale, with random Fe/Co neighbourhoods of the 57 Fe atoms.Mössbauer effect spectra for the Tb 0.27Dy0.73(Fe1−xCox)2 series at room temperature are composed of a number of locally originated subspectra due to the random distribution of Fe and Co atoms in the transition metal sublattice, and due to [1 1 1] an easy axis of magnetization. Isomer shift, magnetic hyperfine field and quadrupole interaction parameter were obtained from the spectra, both for the local area and for the bulk sample.As a result of Fe/Co substitution, a Slater-Pauling-type curve for the average magnetic hyperfine field vs. Co content was observed. It was found that the magnetic hyperfine fields corresponding to the local area also create a dependence of the Slater-Pauling-type vs. Co contribution in the Fe/Co neighbourhoods.