Electrophoretic deposition (EPD) was utilized as a new method for the preparation of hydrotalcite (HT) thin films. The films were deposited on macroporous alumina substrates and on alumina substrates that had been previously coated by conventional dip-coating techniques using slurries of HT colloidal particles. Their permeation properties were investigated by single- and mixed-gas permeation tests, and the films were shown to be permselective toward CO2, which is consistent with prior studies of these materials, which show them to be effective CO2 adsorbents.