Layered clay has been of great interest because of their nano-sized layer structure and hence intercalation and ion-exchange capacity to be used as a host material of composite with polymers and/or metals. In this study, smectite as a silicate-layered clay was easily exfoliated and dispersed into purified water, and was deposited onto a cupper plate for which dc voltage ranging from + 1.0 V to + 6.0 V was applied with respect to a counter platinum plate electrode. The cupper plate was pre-treated by chemical and chemical mechanical polishing (CP and CMP) prior to the electrophoretic deposition (EPD). The surface roughness of the substrate as well as the smectite film formed was characterized by an atomic force microscope (AFM). The thickness of smectite layer was estimated using an X-ray fluorescence (XRF) analysis as well as a scanning electron microscope (SEM) observation. The layer thickness can be described as a function of operational parameters such as applied voltage and operating time. Smooth smectite film with thickness ranging from 100 nm to 10 μm has been successfully fabricated onto the CMP cupper plate by the EPD method in this study.