Atherosclerosis, a chronic inflammatory disease of the arteries, remains a leading cause of death worldwide despite significant advances in treatment over the past several decades. Detailed studies reveal inextricable links between atherosclerosis progression and its underlying pathobiology, ultimately leading to clinical complications of acute myocardial infarction, stroke, ischemic limbs, and sudden cardiac death. Based on a molecular and cellular framework, molecular imaging technologies have made progress in closing the “translational gap” by unraveling fundamental details underlying the in vivo pathogenesis of atherosclerosis not only experimentally, but in humans. In conjunction with high-resolution hardware detection systems, atherosclerosis molecular imaging agents for nuclear imaging, magnetic resonance imaging, optical imaging, computed tomography, and ultrasound imaging show substantial capabilities to decipher a range of key biological targets in vivo and in patients. Here we present state-of-the-art applications of molecular imaging technology to atherosclerosis in the biological, translational, and clinical arenas. As detailed in this chapter, all aspects of atherogenesis from initiation through plaque evolution and ultimately thrombotic complication offer potential targets for molecular imaging by exploiting the pathobiological underpinnings of this disease made over the past two decades.