Nanotechnologies have provided new methods for the preparation of nanomaterials with well-defined sizes and shapes, and many of those procedures have been recently implemented for applications in heterogeneous catalysis. The control of nanoparticle shape in particular offers the promise of a better definition of catalytic activity and selectivity through the optimization of the structure of the catalytic active site. This extension of new nanoparticle synthetic procedures to catalysis is in its early stages, but has shown some promising leads already. Here, we survey the major issues associated with this nanotechnology–catalysis synergy. First, we discuss new possibilities associated with distinguishing between the effects originating from nanoparticle size versus those originating from nanoparticle shape. Next, we survey the information available to date on the use of well-shaped metal and non-metal nanoparticles as active phases to control the surface atom ensembles that define the catalytic site in different catalytic applications. We follow with a brief review of the use of well-defined porous materials for the control of the shape of the space around that catalytic site. A specific example is provided to illustrate how new selective catalysts based on shape-defined nanoparticles can be designed from first principles by using fundamental mechanistic information on the reaction of interest obtained from surface-science experiments and quantum-mechanics calculations. Finally, we conclude with some thoughts on the state of the field in terms of the advances already made, the future potentials, and the possible limitations to be overcome.