Atherosclerosis is a systemic vascular disease predominantly affecting the intima of central and peripheral arteries. Its complications, myocardial infarction and stroke, remain the leading cause of morbidity and mortality in the Western world and developing countries. Angiographic imaging methods are the current gold standard for the clinical graduation of coronary and carotid artery disease and the guidance of treatment. These techniques are however limited to the assessment of the extent of luminal narrowing. MRI is a noninvasive modality, which allows the direct evaluation of the thin arterial vessel wall with excellent soft tissue contrast and high spatial resolution. Targeted MR contrast agents enable the evaluation of specific cellular and subcellular markers on a molecular level. This review will introduce and discuss novel molecular MR imaging techniques for the assessment of plaque and inflammatory burden in the context of atherosclerosis. Both measures can provide additional information beyond the assessment of luminal stenosis alone.