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Cobalt electrodeposits have been produced in chloride solutions. Depending on the electrolysis parameters applied, two different structures for the electrodeposits, namely α and β cobalt were observed. Their characterization included hydrogen content measurement, the relative volume fraction of the α and β phases determined by X-ray diffraction, X-ray diffraction line profile analysis and microstructural investigation by optical microscopy, scanning electron microscopy and transmission electron microscopy. The influence of structure on mechanical properties was examined. The results showed that the ductility properties of the cobalt electrodeposits were highly sensitive to the structure. A higher β phase content that was measured in some deposits did not improve the ductility due to the existence of trapped hydrogen which always exists in such deposits. However, annealing treatments seem to be a promising route to optimize the ductility of cobalt electrodeposits.