Ultraviolet photoelectron spectroscopy of epitaxial films of squaric acid (H2C4O4), a two-dimensional antiferroelectric organic material, is reported. The band structure parallel to the two-dimensional molecular plane was derived, in which the dispersion of the HOMO-2 band was found to be as large as 0.7 eV. The molecular orientation was estimated by analyzing the angular distribution of the photoelectron intensities from various molecular orbitals using independent atomic center approximation.