Microstructures of electrodeposited ni were studied from the perspective of growth modes during electrodeposition. the electrodeposited ni had a heterogeneous microstructure composed of nanocrystalline-and microcrystalline-grains. Electron backscatter diffraction analyses showed that nanocrystalline-and microcrystalline-grains were preferentially oriented to specific planes. Secondary ion mass spectrometry also revealed that coarse-grained regions had higher S content than that of finer-grained regions. Hence, microstructural heterogeneity in electrodeposited Ni is reflected by the overlap of inhibited and free growth modes. our discussion surrounding microstructural heterogeneity also provides insight into other electrodeposited nanocrystalline systems. Nanocrystalline materials often exhibit more favorable properties than coarse-grained materials because of their nano-grain structure 1-3. Electrodeposition is a typical process for fabricating nano-grain structures 4. In practice, Ni and its alloys are electrodeposited with grain sizes below 100 nm 5-8 , and these electrodeposited nanocrystalline metals and alloys show high strength and good ductility 9-13. However, electrodeposited materials have fiber-like textures, which reflect the preferred crystallographic orientation of their crystallites along the growth direction 14,15. The texture formation of electrodeposits is determined by the electrodeposition conditions 16-18. Amblard et al. 19 explained that electrodeposition conditions change the growth mode during electrodeposition. Furthermore, they showed three types of growth modes, namely free-lateral growth, inhibited-lateral growth, and inhibited-out growth, and indicated that each growth mode resulted in specifically oriented textures on electrodeposited Ni. In the few cases where growth modes (or texture) have been considered 12,20,21 , these features have been shown to profoundly affect the microstructure and mechanical properties. Godon et al. 20 reported the relationship between grain orientation and the Hall-Petch relationship in electrodeposited Ni. The Hall-Petch plot of hardness was classified into three regions based on specific textures. In a subsequent report 21 , they found that grain refinement and changes of textures were linked with an increase in impurity content. The incorporation of impurities resulted from the inhibited growth mode. Matsui et al. 12 found a relationship between the tensile elongation and orientation index for the (200) plane in electrodeposited nanocrystalline Ni-W alloys. This relationship indicates that the free-lateral growth mode is suitable for producing ductile electrodeposited nanocrystalline materials. In previous studies 12,20,21 , the effects of growth modes have been discussed by comparison of typical samples having different dominant orientations. These comparisons are based on the assumption that typical samples are electrodeposited by a single growth mode. Contrary to this assumption, our belief is that the actual electrodeposited samples form with multip...