Graphene not only possesses interesting electrochemical behavior but also has a remarkable surface area and mechanical strength and is naturally abundant, all advantageous properties for the design of tailored composite materials. Graphene-semiconductor or -metal nanoparticle composites have the potential to function as efficient, multifunctional materials for energy conversion and storage. These next-generation composite systems could possess the capability to integrate conversion and storage of solar energy, detection, and selective destruction of trace environmental contaminants or achieve single-substrate, multistep heterogeneous catalysis. These advanced materials may soon become a reality, based on encouraging results in the key areas of energy conversion and sensing using graphene oxide as a support structure. Through recent advances, chemists can now integrate such processes on a single substrate while using synthetic designs that combine simplicity with a high degree of structural and composition selectivity. This progress represents the beginning of a transformative movement leveraging the advancements of single-purpose chemistry toward the creation of composites designed to address whole-process applications. The promising field of graphene nanocomposites for sensing and energy applications is based on fundamental studies that explain the electronic interactions between semiconductor or metal nanoparticles and graphene. In particular, reduced graphene oxide is a suitable composite substrate because of its two-dimensional structure, outstanding surface area, and electrical conductivity. In this Account, we describe common assembly methods for graphene composite materials and examine key studies that characterize its excited state interactions. We also discuss strategies to develop graphene composites and control electron capture and transport through the 2D carbon network. In addition, we provide a brief overview of advances in sensing, energy conversion, and storage applications that incorporate graphene-based composites. With these results in mind, we can envision a new class of semiconductor- or metal-graphene composites sensibly tailored to address the pressing need for advanced energy conversion and storage devices.