Despite the fact that technological advancements have been made in diagnosis and treatment, cardiovascular diseases (CVDs) remain the leading cause of mortality and morbidity worldwide. Early detection of atherosclerosis (AS), especially vulnerable plaques, plays a crucial role in the prevention of acute coronary syndrome (ACS). Targeting the critical cytokines and molecules that are upregulated during the biological process of AS by in vivo molecular imaging has been widely used in plaque imaging. With their three-dimensional architecture, composition, and abundant terminal functional groups, dendrimers provide a platform for multitargeting and multimodal imaging. Thus, modified dendrimers with the key molecules upregulated in AS plaques will be an innovative attempt to achieve targeted imaging of AS plaques specifically and efficiently. This review was aimed to address some recent works on imaging of AS plaques using various types of image technology and further discuss the applications of dendrimers, an innovative yet seldom used method in imaging of AS plaques due to some limitations and challenges, and we highlight the bright future of the modified dendrimers in characterizing AS plaques.