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Electrogalvanized steel sheets coated with thin organic films containing silica have been utilized for electrical home appliances because they have excellent resistance to fingerprints and corrosion. It is important to control the crystal orientation of zinc as it affects the lightness,1,2) glossiness,1) surface roughness,3,4) and press formability4,5) of the electrogalvanized steel sheets. Therefore, there have been numerous studies regarding how the orientation is affected by electrolysis conditions,3,6–9) types of electrolytes,10,11) addition of inorganic12–14) and organic15–18) compounds to the solutions, and preadsorption19–22) of organic additives onto the iron substrate. During Zn deposition on an α–Fe substrate, the initial Zn deposits grow epitaxially, according to Burgers’ orientation relationship, which is described as {110}Fe//{0001}Zn and [111]Fe//[1120]Zn.10,23) In addition, the deposits are reported to epitaxially grow according to the relationship of Effect of Surface Textures of Iron Substrate on the Crystal Orientation Relationship between Electrodeposited Zinc and Iron