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Simple Summary: Cardiovascular diseases are the first cause of morbimortality worldwide. They are mainly caused by atherosclerosis, with progressive plaque formation in the arterial wall. In this context, several imaging techniques have been developed to screen, detect and quantify atherosclerosis. Early screening improves primary prevention and promotes the prescription of adequate medication before adverse clinical events. In this review, we focus on the imaging of vascular cell adhesion molecule-1, an adhesion molecule involved in the first stages of the development of atherosclerosis. This molecule could therefore be a promising target to detect early atherosclerosis non-invasively. Potential clinical applications are critically discussed.