Dual-energy computed tomography (CT) combines the high spatial resolution of standard CT with the ability to improve contrast resolution, reduce artifact, and separate materials of different atomic weights and energy-based attenuation through postprocessing. We review the underlying physical principles and applications of dual-energy CT within the context of patients undergoing preprocedural and postprocedural evaluation for neurointerventional therapies. The broad imaging categories of cerebral ischemia and hemorrhage, head and neck angiography, and the spine are reviewed.