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Despite intensive therapy regimen, brain cancers present with a poor prognosis, with an estimated median survival time of less than 15 months in case of glioblastoma. Early detection and improved surgical resections are suggested to enhance prognosis; several tools are being explored to achieve the purpose. Raman spectroscopy (RS), a nondestructive and noninvasive technique, has been extensively explored in brain cancers. This review summarizes RS-based studies in brain cancers, categorized into studies on animal models, ex vivo human samples, and in vivo human subjects. Findings suggest RS as a promising tool which can aid in improving the accuracy of brain tumor surgery. Further advancements in instrumentation, market-assessment, and clinical trials can facilitate translation of the technology as a noninvasive intraoperative guidance tool.