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Peripheral vascular disease (PVD) is an atherosclerotic disease affecting the lower extremities, resulting in skeletal muscle ischemia, intermittent claudication, and, in more severe stages of disease, limb amputation and death. The evaluation of therapy in this patient population can be challenging, as the standard clinical indices are insensitive to assessment of regional alterations in skeletal muscle physiology. Radiotracer imaging of the lower extremities with techniques such as PET and SPECT can provide a noninvasive quantitative technique for the evaluation of the pathophysiology associated with PVD and may complement clinical indices and other imaging approaches. This review discusses the progress in radiotracer-based evaluation of PVD and highlights recent advancements in molecular imaging with potential for clinical application.