Sm-Co alloys as permanent magnetic materials have attracted considerable interest for their application in the miniaturization of electronic devices. However, a facile method for depositing SmCo alloy films is still urgently needed. In this work, we exploited a simple aqueous electrodeposition approach to prepare Sm-Co films. Electrodeposition was realized by galvanostatic electrolysis from a stable sulfamate aqueous solution. The influence of the applied current density on the composition, morphology, structure and magnetic properties of the Sm-Co films was studied. Samarium was successfully incorporated into the films by the induced effect of Co(II) ions. Manipulating the current density varied the samarium content from 5.8 to 25.3 at%. Sm-Co nanosheets were discovered and were determined to have a mixed nanocrystalline/amorphous character. Furthermore, the electrodeposited Sm-Co films exhibited an obviously enhanced coercivity compared with that of other reported films.