Carotid atherosclerotic disease is a significant preventable cause of stroke. Clinical decision-making in current practice is based primarily on detection of the severity of luminal stenosis, as determined by ultrasound or conventional angiographic imaging modalities. New insights in the biology of atherosclerosis now suggests that the morphological characteristics of the carotid plaque as well as the molecular and cellular processes occurring within it may be more important markers of plaque vulnerability and stroke risk. This review summarizes emerging applications in the molecular imaging of atherosclerosis and detection of the vulnerable carotid plaque. We discuss how advances in imaging platforms and biochemical technology (e.g. targeted contrast agents) have driven some exciting and promising novel diagnostic imaging approaches from bench to bedside.