The preparation of the metal surface before coating application is fundamental in determining the properties of the coatings, particularly the roughness, adhesion, and corrosion resistance. In this work, chitosan/Eudragit E 100 (chit/EE100) were fabricated by electrophoretic deposition (EPD) and both their microstructure and properties were investigated. The present research is aimed at characterizing the effects of the surface pretreatment of titanium substrate, applied deposition voltage, and time on physical, mechanical, and electrochemical properties of coatings. The coating’s microstructure, topography, thickness, wettability, adhesion, and corrosion behavior were examined. The applied process parameters influenced the morphology of the coatings, which affected their properties. Coatings with the best properties, i.e., uniformity, proper thickness and roughness, hydrophilicity, highest adhesion to the substrate, and corrosion resistance, were obtained after deposition of chit/EE100 coating on nanotubular oxide layers produced by previous electrochemical oxidation.