Well-ordered two-dimensional thin films can now be routinely produced by either vacuum deposition and/or self-assembly deposition technologies, and rules for epitaxial growth of such materials on a variety of single crystal substrates are becoming well understood. This talk will review recent work on the growth of both phthalocyanine and perylene dye thin films, on both single crystal metal and nonmetal surfaces. Many of the crystalline organic dyes tend to form flat-lying ordered monolayers, with coincident epitaxial relationships with the substrate. Several interesting cases have recently emerged, however, where such flat-lying monolayers are not formed, and/or where neither coincident nor commensurate epitaxial structures are formed, but ordered films result nevertheless. In all events organic heterojunction formation is of interest for these materials, and characterization of such heterojunctions by combinations of XPS/UPS will be discussed. In addtion, we will discuss recent self-assembly approaches to ordered phthalocyanine thin films, by non-vacuum deposition approaches, which produce coherence in thin film structures rivaling the best vacuum deposited materials.