Nanocrystalline materials are of technological importance due to their interesting properties such as their ductility, high strength, wear resistance and magnetic properties. Because of their attractive properties, there has been great emphasis on studying these materials. Many synthesis techniques have been developed such as gas condensation, ball-milling, chemical processing, sol-gel technique, sputtering, rapid solidification and electrodeposition. Among the methods mentioned above, electrodeposition is considered to have more eligibility because of some advantages. In this method, the deposition can be proceeded under the normal condition of temperature and pressure which results in better control of process and lower costs for the equipments. Production and characterization of nanocrystalline iron-nickel alloys have been received a lot of attentions due to their interesting mechanical and magnetic properties. The Fe-Ni alloys fabricated by electrodeposition are used in the electronic industries for memory, recording and storage devices, NEMS/MEMS and low CTE applications. In this study, nanocrystalline Fe-Ni alloys were produced by electrodeposition. Free-additive chloride baths were used to lessen the impurities in produced alloys. The influence of bath concentration, current density and pulse current density was studied. The chemical composition of alloys was determined by EDS semi-quantitative analysis. The investigations showed that the Fe content increased with decrease in Ni/Fe ion ratio but the relationship is not linear. This is because of anomalous co-deposition behavior of Fe-Ni system. For the deposits with high iron content, the structure was in the form of bcc. With increase of Fe content to about 60-70%, a dual phase alloy consisting of bcc and fcc crystal structures was formed. Further increase in Fe content resulted in the formation of a single phase with fcc crystal structure. Due to XRD patterns and previous studies, the formation of FeNi 3 intermetallic compound was also possible in this method. The average grain size of Fe-Ni alloys was about 8-16 nm which was increased with decrease of Fe content of the alloy. Also, an increase in current density led to higher content of Ni and coarser grains. Applying high frequency pulse current density led to the increase in Fe content and decrease in grain size. The hardness of deposits increased with decrease in grain size which was in consistent with Hall-Petch relationship. The study of magnetic properties of deposits by AGFM analysis showed an increase in saturation magnetization with increase in Fe concentration of bath and applying pulse current. In addition, a decrease in grain size led to lower coercivity, although, the Fe content of deposits increased. Keywords: Electrodeposition; Fe-Ni alloys; Nanostructures; Soft magnetic material