Optical Coherence Tomography (OCT) has emerged as a transformative imaging modality, offering high-resolution, cross-sectional imaging of tissue microstructure. Diagnosis of cerebrovascular disease involves a range of vascular neuroimaging techniques, including computed tomography (CT) angiography, magnetic resonance (MR) angiography (with or without contrast agents), and catheter digital subtraction angiography (DSA). These modalities primarily focus on providing information about the vessel lumen. Currently available OCT systems face challenges in being used routine within the intracranial circulation due to vessel caliber and tortuosity. Current endovascular treatments for brain vessel pathologies rely on image guidance with limited resolution, hindering thorough assessment of underlying arterial conditions and therapeutic devices. High-resolution imaging capable of visualizing cerebral artery microstructure and neurovascular device features could revolutionize cerebrovascular disease research, diagnosis, and treatment. The neurovascular high-frequency optical coherence tomography (HF-OCT) system, designed to rapidly capture volumetric microscopy data with resolutions nearing 10 microns in tortuous cerebrovascular anatomies. The potential of HF-OCT for cerebrovascular imaging was evaluated and demonstrated through multiple in vitro, ex vivo, and in vivo models.