This report describes methods to produce large-area films of graphene oxide from aqueous suspensions using electrophoretic deposition. By selecting the appropriate suspension pH and deposition voltage, films of the negatively charged graphene oxide sheets can be produced with either a smooth "rug" microstructure on the anode or a porous "brick" microstructure on the cathode. Cathodic deposition occurs in the low pH suspension with the application of a relatively high voltage, which facilitates a gradual change in the colloids' charge from negative to positive as they adsorb protons released by the electrolysis of water. The shift in the colloids' charge also gives rise to the brick microstructure, as the concurrent decrease in electrostatic repulsion between graphene oxide sheets results in the formation of multilayered aggregates (the "bricks"). Measurements of water contact angle revealed the brick films (79°) to be more hydrophobic than the rug films (41°), a difference we attribute primarily to the distinct microstructures. Finally, we describe a sacrificial layer technique to make these graphene oxide films free-standing, which would enable them to be placed on arbitrary substrates.