In spite of a great improvement in medical health services and an increase in lifespan, we have witnessed a skyrocket increase in the incidence of central nervous system (CNS) disorders including brain tumors, neurodegenerative diseases (Alzheimer's disease, Parkinson's disease, amyotrophic lateral sclerosis, Huntington's disease), ischemic stroke, and epilepsy, which have seriously undermined the quality of life and substantially increased economic and societal burdens. Development of diagnostic methods for CNS disorders is still in the early stage, and the clinical outcomes suggest these methods are not ready for the challenges associated with diagnosis of CNS disorders, such as early detection, specific binding, sharp contrast, and continuous monitoring of therapeutic interventions. Another challenge is to overcome various barrier structures during delivery of diagnostic agents, especially the blood-brain barrier (BBB). Fortunately, utilization of nanomaterials has been pursued as a potential and promising strategy to address these challenges. This review will discuss anatomical and functional structures of BBB and transport mechanisms of nanomaterials across the BBB, and special emphases will be placed on the state-of-the-art advances in the development of nanomedicines from a variety of nanomaterials for diagnosis of CNS disorders. Meanwhile, current challenges and future perspectives in this field are also highlighted. Copyright © 2020 Elsevier Ltd. All rights reserved.