Positron emission tomography (PET) provides a non-invasive method to measure biological processes that are relevant to atherosclerosis, including arterial inflammation and calcification. The vast majority of studies imaging atherosclerosis with PET have utilized the tracer 18F-fluorodeoxyglucose (FDG) to better understand how inflammation contributes to atherosclerosis development, and to test the efficacy of therapeutic interventions aimed at reducing its progression. Additional tracers such as 18F-sodium fluoride (18F-NaF) provide additional avenues for characterizing atherosclerosis development. This review examines the emerging uses of PET arterial imaging as a marker of vascular inflammation and atherosclerosis, as a prognostic tool, and as a clinical research tool. In addition, we examine emerging methods that should advance arterial imaging with PET.