Low-dimensional materials functioning at the nanoscale are a critical component for a variety of current and future technologies. From the optimization of light harvesting solar technologies to large-scale catalytic processes, key physical phenomena are occurring at the nanometer and atomic length-scales and predominately at interfaces. For instance, graphene is a nearly ideal two-dimensional conductor that is comprised of a single sheet of hexagonally packed carbon atoms. In order fully realize the potential of graphene for novel electronic applications, large-scale synthesis of high quality graphene and the ability to control the electronic properties of this material on a nanometer length scale are key challenges. In addition to graphene, we are interested in exploring the synthesis of low-dimensional materials that do not occur in nature. This talk will highlight how scanning probe microscopy presents a series of powerful experimental tools that can overcome several challenges and allow for the direct characterization of several advanced materials. This talk will also cover our most recent discovery and synthesis of new two-dimensional (2D) boron allotropes (borophenes). This discovery of metallic 2D sheets of boron presents almost ideal example of the synergy between predictive modeling resulting in the experimental realization of a designer materials.