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In recent years, there has been advancement in the management of primary and secondary brain tumors within a multidisciplinary framework. However, substantial challenges persist in optimizing treatment strategies, enhancing survival rates, and improving patient prognosis and quality of life. These challenges stem from the complex interplay of biological processes that drive tumor pathogenesis and encompass factors such as tumor heterogeneity and patient variability together with surgical access and resectability in certain brain areas. Current therapeutic modalities – surgical resection, radiotherapy, and systemic pharmacotherapy – all have their own inherent limitations. However, promising alternative treatments are seen in emerging techniques such as endovascular radiosurgery, specifically ones that use intra-arterial delivery of radioactive Yttrium-90 (90Y) microspheres. This approach is currently used in hepatocellular carcinoma (HCC) treatment, which allows for the precise and targeted delivery of radiation to the tumor while minimizing systemic toxicity. Advances in imaging modalities such as MRI and single-photon emission computerized tomography (SPECT)/CT facilitate accurate dosimetry planning and ensure optimal therapeutic outcomes. This review provides the first comprehensive synthesis of the rationale, technical considerations, and translational potential of 90Y-based endovascular radiosurgery in neuro-oncology. While intra-arterial therapies and radiotherapy are established in other fields, their convergence for intracranial applications—particularly in bypassing the blood-brain barrier (BBB) and achieving localized brachytherapy—remains in its early preclinical and clinical stages. We highlight specific central nervous system (CNS) use cases, preclinical findings, and procedural adaptations needed for this modality’s advancement in brain tumor care.