Surface science continues as an exciting frontier—perhaps more so now than in the past—for at least two reasons. First, powerful new tools are emerging, and second, a broad and robust body of knowledge has been established which is serving as a springboard for new breakthroughs, and is critically guiding other fields. In this talk I will present some of the contributions that I and my coworkers have been privileged to make in this field, particularly in the area of quasicrystal surfaces, and in the area of growth and stability of nanoclusters and thin films at surfaces. Metallic quasicrystals have a remarkable atomic structure that engenders unusual properties, including surface properties, and our goal has been to establish the structure-property relationship at the surface. One of our achievements was to show that quasicrystal surfaces are generally bulk-terminated. This laid the groundwork for showing that one of the characteristics of quasicrystals—low friction—derives (at least in part) from the quasiperiodic atomic structure. It also allowed us to understand unusual features of thin film nucleation and growth on these surfaces, and facilitated efforts of other groups to exploit quasicrystals and complex metallic alloys as catalysts. Nucleation and growth of nanoclusters and thin films also shows surprising features on more conventional (crystalline metal) surfaces, and has been a topic of investigation in my group for some time. We discovered that unusual smooth growth at low temperature, and associated non-monotonic temperature dependence of roughness, reflects a process now called “downward funneling”. In addition to non-equilibrium growth morphologies, we have also explored the relaxation of these morphologies towards equilibrium. We found that two-dimensional homoepitaxial metal nanoclusters can diffuse significant distances, leading to coarsening (a reduction in the cluster density) via agglomeration. Nanocluster destabilization and coarsening can also occur via Oswald ripening, but the identity of the mass carriers may not be obvious. The presence of even trace amounts of adsorbates can lead to formation of additive-metal complexes which more efficiently transport mass than metal atoms. We have searched for these complexes under conditions which have rarely been investigated in the past, i.e. very low temperature and very low coverage, with some surprising results.